Lithium is a vital strategic resource for the modern energy transition. However, conventional adsorption methods are limited by slow extraction kinetics and substantial freshwater consumption. In this work, a lithium-extracting hydrogel (LEH) driven by a novel charge-transfer (CT) organic cocrystal (ATQ) is developed for interfacial solar evaporation-driven lithium extraction. ATQ cocrystals exhibit strong CT interactions, panchromatic absorption, and a high photothermal conversion efficiency of 90.27 +/- 0.85% at 1550 nm, efficiently harnessing the energy within the near-infrared II (NIR-II) region of the solar spectrum. The LEH hydrogel is optimized through structure design, achieving an evaporation rate of 2.48 kg m-2 h-1. Evaporative flow-driven convection suppresses the concentration polarization of protonated lithium titanate (HTO) and accelerates ion transport. Localized interfacial heating enhances adsorption kinetics, enabling efficient lithium extraction. The LEH demonstrates a Li+ adsorption capacity of 23.4 mg g-1 in simulated solution under 1 Sun and exhibits superior Li+/Mg2+ selectivity with a separation factor of approximately 180 in high-magnesium brines. Importantly, the collected condensate can be reused as the water source for preparing acidic eluent for Li+ stripping, enabling condensate-assisted regeneration of the LEH. This integrated strategy highlights the potential of coupling solar-driven lithium extraction with freshwater co-generation to reduce freshwater demand in salt lake lithium recovery.

The development of high-performance blue OLEDs with narrowband emission, high efficiency, and high stability is crucial for ultrahigh-definition displays. The limitations of amorphous films, notably their low carrier mobility and inherent instability, pose significant impediments to the development of OLED technology. To address this challenge, a p-type organic single crystal (SC) of 3PV-Me with favorable crystalline and optoelectronic properties was introduced in the OLEDs (SC-OLEDs) as the hole transport layer (HTL) in combination with an emissive layer (EML) consisting of a triplet-triplet up-conversion (TTU) host doped with multi-resonant thermally activated delayed fluorescence (MR-TADF) blue emitters. Through a systematic investigation, 3PV-Me SC-HTLs are demonstrated to exhibit superior interfacial characteristics at both the SC-HTL/EML and SC-HTL/electrode interfaces, thereby facilitating highly ordered crystallinity of the EML with a higher horizontal dipole ratio. Benefiting from these advantages, the fabricated SC-OLEDs achieve a pure-blue emission with a full width at half maximum (FWHM) of only 23 nm and a y color coordinate below 0.07, alongside a high external quantum efficiency (EQE) exceeding 10.02%, and long operational lifetime (LT50 > 1076 h). These findings highlight the significant potential of the SC-HTL strategy for realizing efficient and stable blue OLEDs with high color purity.

The extreme sensitivity to the environment and inherent instability of organic materials have posed persistent challenges to achieving long-term operational stability of organic light-emitting diodes (OLEDs). Herein, a dual-functional single-crystalline layer of 1,4-bis(4-methylstyryl)benzene (BSB-Me) is introduced into the OLED structure, simultaneously serving as both an intrinsically stable hole-transporting layer (HTL) and an effective barrier layer, to improve device stability. Systematic characterizations are conducted to gain an insight into the stability property of BSB-Me single crystals (SCs), confirming their robust thermal, morphological, and electrochemical stabilities. The SCs also exhibit desirable barrier property with a low water vapor transmission rate (WVTR) of approximately 3.58 × 10-4 g m-2 day-1, which is comparable to that of a 50-nm-thick monolayer Al2O3 barrier layer. In consequence, highly efficient and stable single-crystal OLEDs (SC-OLEDs) can be successfully fabricated by introducing the dual-functional BSB-Me SC layer. The blue SC-OLEDs present extended operational lifetimes (LT75) of over 1209 h at an initial luminance of 1000 cd cm-2, which is notably more than thirty times enhanced compared to that of conventional OLEDs with amorphous HTLs. Our findings suggest that the introduction of a dual-functional single-crystalline layer presents a promising advancement for improving the operational stability of OLEDs.

Two-dimensional in-plane molecular superlattice heterojunctions, where distinct semiconducting components are integrated laterally within a single crystalline plane, offer an ideal architecture for controlling charge separation and transport in optoelectronic devices. However, realizing such structures with molecular-level precision, long-range periodicity, and sharp interfaces in organic semiconductors remains a major challenge. Here, the first 2D organic heterojunction featuring long-range, in-plane donor-acceptor superlattice via cocrystal engineering is presented. By employing phase-separated molecular design for the donor (TIPS-PEN) and acceptor (PDI-FCN), strong in-plane cohesion is decoupled from out-of-plane steric repulsion, inducing a periodic -D-A-D- arrangement within the crystal plane. The resulting high-density, lattice-defined heterointerfaces facilitate exciton dissociation, directional charge transport, and efficient extraction. The ultrathin crystal enables effective gate-field control, yielding ambipolar OFETs with exceptional on/off ratios of 108 (holes) and 107 (electrons). Capitalizing on the narrow bandgap and the ordered 2D heterointerface, this material demonstrates outstanding high-energy photon conversion efficiency. As an X-ray detector, it exhibits high sensitivity of 4.21 × 104 µC Gy-1 cm-2 and low detection limit 5.73 nGy s-1, enabling clear imaging at 14.77 nGy s-1 ultralow dose rate. This work provides new ideas for constructing 2D multicomponent organic heterostructures and unlocks potential for next-generation flexible electronics and low-dose radiation sensing.

Despite their significant potential in advanced display and lighting applications, the commercialization of white organic light-emitting diodes (WOLEDs) is still hindered by the intrinsic complexity of their multi-layer device structures and material systems. Here, we demonstrate an all-in-one single-crystalline layer, simultaneously serving as the emissive layer (EML), hole-transport layer (HTL), and moisture barrier layer (MBL), can effectively overcome these limitations. TBU-DNA single crystals (SCs) inherently possess strong blue fluorescence emission of an EML, high hole mobility of an HTL, and robust moisture permeation barrier ability of an MBL. By harnessing these triple synergistic functions, we fabricate a three-organic-layer WOLED that achieves a maximum current efficiency of 22.1 cd A-1 and EQE of 7.6%. These features represent the highest reported values for WOLEDs fabricated from organic single-crystalline materials. The inherent barrier property of the TBU-DNA SCs endows the device with remarkable operational stability, achieving a lifetime (LT80) of 649 h at an initial luminance of 1000 cd m-2. Through a precise manipulation of the exciton recombination zone, the single-crystal WOLEDs exhibit a high CRI of 86 and a color temperature of 5580 K. The multifunctional TBU-DNA single crystals represent a significant advance toward structurally simplified, high-performance white OLEDs for practical applications.

The International Roadmap for Devices and Systems (IRDS) has identified the tunnel field-effect transistor (TFET) as the most promising next-generation logic device that enables sustainable downscaling in driving voltage and power consumption. Demonstrating an acceptable sub-Boltzmann-limit ON current (namely I60, the current level when a TFET switches to a subthreshold swing level of 60 millivolts per decade) and current-switching ratio has presented a formidable challenge. We report a TFET based on a bismuth/indium selenide (Bi/InSe) heterostructure that exhibits an I60 of up to ~10 microamperes per micrometer and a current-switching ratio of >107. We attribute such promising TFETs to precise material design, clean interfaces fabricated under vacuum, and band engineering based on subthreshold swing physics. Our results demonstrate a high-performance basic building block that meets the IRDS requirements for next-generation integrated circuits.

Two-dimensional organic molecular crystals (2DOMCs) have emerged as promising candidates for next-generation ultrathin electronics. However, precisely and reversibly modulating their charge-transport characteristics remains a significant challenge. Herein, we report a molecular engineering strategy to create light-programmable field-effect transistors (FETs) based on a monolayer thick 2DOMCs, which is achieved by dispersing photochromic diarylethene (DAE) guests into a crystal host matrix of 2,6-bis(4-hexylphenyl) anthracene (C6-DPA). By systematically functionalizing the DAE periphery with substituents of varying electron-donating and -withdrawing strengths, we precisely tune the HOMO energy levels of the guest molecules. We identify DAE-OCH3 as the optimal dopant, which enables a 54% modulation of the FET current within just 5 s of UV light "writing" process. Notably, the optimized C6-DPA/DAE-OCH3 (15%) guest-host system exhibits approximately 85 distinct and stable current levels, corresponding to a storage capacity exceeding 6 bits, with excellent retention over 16 days. This performance represents a significant advancement in ultrathin multilevel memories based on high-mobility organic semiconductors. Our approach establishes a general platform for developing stimuli-responsive 2D organic materials with programmable (opto)electronic properties, opening new avenues for high-density data storage and future generation intelligent (opto)electronics.

Organic single crystals (SCs) are promising candidates for high‐performance optoelectronic devices due to their high mobility of charge carriers and oriented alignment of transition dipole moments (TDMs). However, organic single‐crystal‐based light‐emitting diodes (SC‐based OLEDs) have until now struggled with poor device efficiency because of the lack of appropriate SC emitters; the integration of superior charge‐transport property and light‐emitting behavior into one single SC remains a great challenge. Here, two anthracene‐derivative SCs, 2,6‐di(6‐ tert ‐butylnaphthyl)anthracene (TBU‐DNA) and 2,6‐di(2‐naphthyl)anthracene (2,6‐DNA), are introduced into the construction of high‐efficiency SC‐based OLEDs. Through systematic investigations, rational crystal packing is revealed to play a critical role in tailoring the optoelectronic properties of SCs. Thanks to the slipped herringbone packing motif, TBU‐DNA SC is endowed with a higher photoluminescence quantum yield (PLQY) of 71.47%, an enhanced light‐outcoupling efficiency of 22.9%, and higher charge‐carrier mobility reaching up to 1.44 cm 2 V −1 s −1 along the crystal c ‐axis, which are all responsible for better electroluminescence (EL) performances of TBU‐DNA SC‐based OLEDs. By optimizing the device structure with a hole‐blocking layer (HBL), the external quantum efficiency (EQE) of TBU‐DNA SC‐based OLEDs is approaching 3.46%, which is one of the highest EQE values for those OLEDs based on the SC emitting layer (EML) reported so far.

Organic semiconductor single‐crystal heterojunctions (OSSCHs) are engineered by integrating complementary organic semiconductor crystals to enable ambipolar transport and multifunctional device performance. This review outlines recent progress in the crystal growth, interface physics, and device applications of OSSCHs, with an emphasis on low‐dimensional structures achieved through controlled crystallization and advanced interface engineering. Innovations in crystallization control, such as integrated self‐assembly and van der Waals epitaxy, have enabled the construction of defect‐minimized heterointerfaces with molecular‐level precision. Emerging strategies in low‐dimensional engineering, including vertically stacked heterostructures and ultrathin 2D molecular crystals, have optimized carrier dynamics while introducing unique optoelectronic properties. The engineered band alignment at heterointerfaces critically governs exciton dissociation efficiency and charge transport pathways, directly enhancing device performance in photovoltaics and light‐emitting systems. These heterojunctions demonstrate promising applications across ambipolar transistors, light‐emitting devices, and neuromorphic electronics by overcoming the inherent limitations of unipolar active layers. The review also highlights current challenges and future research directions, emphasizing the role of OSSCHs in advancing the fields of materials science and optoelectronic device engineering.

When light interacts with diverse media via reflection, transmission, and scattering, its polarization state alters, encoding the spectral information specific to the object's features. With advancements in the smart era, polarization detection is progressing toward miniaturization, integration, and enhanced multifunctionality, where polarization-sensitive active layers are pivotal. Organic semiconductors—featuring chemically tailored photoelectric properties and precisely engineered optical anisotropy, as well as cost-effectiveness and flexibility—emerge as promising candidates for next-generation polarized-light detection. This review highlights the cutting-edge progress of organic-semiconductor–based photodetectors in polarization-sensitive detection. Beginning with a brief introduction to polarization detection, it then summarizes recent developments in organic materials sensitive to linear and circular polarization light, specifically focusing on organic single crystals and aligned conjugated polymers for linear polarization detection; chiral small molecules, chiral conjugated polymers, and chiral supramolecules for circular polarization detection. Advanced applications of these materials, including polarization imaging, biomimetic vision, and information encryption are subsequently discussed. The review concludes by highlighting the prevailing challenges and outlining future research directions essential for advancing high-performance, integrated polarization-sensitive photodetectors in this rapidly evolving field.

ABSTRACTOrganic single crystals with long‐range molecular periodic ordering ensure superior charge‐transport properties and low defect density, which have been considered promising candidates for charge‐transporting materials in organic light‐emitting devices (OLEDs). The functional interfaces of OLEDs play a critical role in charge‐transporting and light‐emitting behaviors, while the interfacial properties of organic single crystals in OLEDs and their impact on device performance have been rarely investigated. Herein, two typical organic single crystals, 1,4‐bis(4‐Methylstyryl)benzene (BSB‐Me) and 2,6‐diphenylanthracene (DPA) with different molecular formulas and packing structures, are introduced as the single‐crystal hole‐transporting layers (HTLs) for a systematic investigation of the interfacial properties between single‐crystal HTLs and active emissive layers. BSB‐Me single‐crystal HTLs offer satisfied surface wettability and enhanced interfacial interaction, which dominate the charge‐transporting and light‐emitting behaviors of the OLEDs. Such improved interfacial properties are responsible for the superior light out‐coupling efficiency of BSB‐Me single‐crystal OLEDs with efficient exciton recombination and minimal Joule heat loss. In consequence, BSB‐Me single‐crystal OLEDs exhibit a maximum luminance of 50,170 cd/m2 and a peak EQE of 8.78%, which are better than DPA‐based devices. Furthermore, BSB‐Me single‐crystal HTLs with favorable interfacial properties enable large‐area OLEDs with uniform EL emission over the whole light‐emitting area of 1 mm × 1 mm.

Ambipolar carrier transport in organic single crystals is essential to maximize exciton recombination and thus achieve high-efficiency organic light-emitting diodes (OLEDs). Herein, two bis-styrylbenzene derivatives, 1,4-bis(4-methylstyryl)benzene (3PV-Me) and 1,4-bis(4-trifluoromethylstyryl)benzene (3PV-CF3), are introduced into the construction of ambipolar 3PV-CF3 doped 3PV-Me (3PV-Me-CF3) single crystals. The same molecular skeleton of these two molecules endow them with similar molecular shapes and sublimation temperatures. Doping with 3PV-CF3 dopants is evaluated for their effect on the photophysical properties of host 3PV-Me crystal. Systematic spectroscopic investigations and high-resolution time-of-flight secondary ion mass spectrometry (TOF-SIMS) depth profiling are further conducted to gain a deep insight into the doping details of 3PV-Me-CF3 single crystals. Furthermore, their ambipolar carrier transport behavior is evaluated by the space-charge-limited current (SCLC) method, exhibiting nearly equal hole and electron mobilities. These ambipolar 3PV-Me-CF3 single crystals are then utilized for the fabrication of single-crystal OLEDs, which demonstrated an almost sixfold enhancement in the electroluminescence (EL) efficiency in comparison to the unipolar 3PV-Me single-crystal OLEDs. The findings reveal the great potential of well-balanced ambipolar organic single-crystalline semiconductors for the development of high-performance single-crystal optoelectronic devices.

Few-layered potassium nickel and cobalt oxides show drastic differences in catalytic activity based on metal ion preorganization. Uniform compositions [(CoO2/K)6 or (NiO2/K)6] show limited activity, while homogeneously mixed-metal cobalt/nickel oxides [(Co n Ni(1-n)O2/K)6] display moderate improvement. However, a layer-by-layer arrangement of alternating cobalt and nickel oxide sheets [e.g., (CoO2/K/NiO2/K)] provides superior catalytic performance, reducing the oxygen evolution overpotential by ∼200-400 mV. Density functional theory simulations provide an illustration of the electronic properties (density of states and localization of orbitals) that promote catalysis in the layer-segregated materials over those of homogeneous composition. This study reveals that atomic preorganization of metal ions within layered catalysts plays a more crucial role than the overall metal composition in enhancing catalytic efficiency for oxygen evolution.

Carbon electrodes effectively address halogen corrosion issues in perovskite devices; however, challenges such as energy level mismatching and solvent corrosion limit their direct application in p-i-n perovskite photovoltaic devices. In this study, a C60/SnOX bilayer was introduced to mitigate solvent corrosion during the fabrication of carbon electrodes. By tailoring the C60/SnOX bilayer, the device performance was significantly enhanced through the formation of a hierarchical energy-level interface. This optimization enabled more efficient charge transport and reduced recombination losses, resulting in a record-breaking efficiency of 21.1% for p-i-n carbon-electrode perovskite photovoltaic cells(CE-PPCs), marking the highest reported efficiency for this device architecture. The device also demonstrates excellent performance under indoor light conditions, with an efficiency of 35.6%. This method also demonstrates excellent scalability, enabling the production of high-performance modules with an aperture area of approximately 20 cm2. The modules achieve an efficiency of 15.1% under 1 sun illumination and 26.3% under indoor lighting conditions. The module also exhibited excellent stability, retaining 96.82% of its initial efficiency after 2218 h of damp-heat aging (85% relative humidity, 85 °C). Under continuous 1 sun illumination at 73 °C in an open-circuit state, the module's efficiency increased to 104.3% after 347 h, whereas devices with Ag electrodes exhibited severe degradation, failing within 96 h.

Significance As one of the most important inventions in the 20th century,the laser has been widely termed"the fastest knife,""the most accurate ruler,"and"the brightest light."A laser represents light amplification by the stimulated emission of radiation,which can explain the lasing generation process.Organic lasers,as important components of lasers,have received extensive attention in the field of optoelectronics for various applications owing to their advantages,such as facile fabrication,low cost,and ease of integration.Recently,organic lasers have been used extensively,and the design and synthesis of a series of promising organic-laser gain media have intensified.The development of optically pumped organic lasers has progressed significantly;however,the aim of electrically pumped organic lasers remains a worldwide research problem.Owing to the three key components of organic lasers,the fabrication of optical resonators is crucial to realize efficient and stable electrically pumped organic lasers. Progress Here,we summarize the recent novel developments of electrically pumped organic lasers,from material selection to device optimization.Three types of optical resonators are typically used in electrically pumped organic lasers:distributed feedback structures(DFBs),distributed Bragg reflectors(DBRs),and whispering gallery mode(WGM).To realize electrically pumped organic lasers,the following criteria must be satisfied:sufficient current injection and exciton densities to induce population inversion,clear threshold behavior of current-density-dependent spectral narrowing and output-power enhancement,and observation of both spatial and temporal coherence.Figure 1 shows the organic four-level system under electrical excitation and the lasing behavior of the output power and FWHM(full width at halt maxima)as a function of current density.In Section 2.1,we summarize the recent developments of electrically pumped organic lasers based on DFB resonators.DFB resonators are considered to be among the most effective structures for realizing electrically pumped organic lasers.They are essentially periodic Bragg-grating structures that can provide effective optical feedback for lasing oscillations via Bragg scattering.Figure 2 illustrates an electrically pumped organic laser with a DFB structure,in which an electroluminescent device incorporates a mixed-order distributed feedback SiO2 grating into an organic light-emitting diode(OLED)structure and emits blue lasing.Figure 3 shows an electrically driven organic laser with an integrated device structure that efficiently couples an OLED with exceptionally high internal-light generation and a polymer-distributed feedback laser.Under electrical driving,a threshold in the light output versus the drive current with a narrow emission spectrum and the formation of a beam above the threshold are observed.Section 2.2 summarizes the recent novel developments of electrically pumped organic lasers based on DBR resonators.DBR resonators are periodic structures comprising alternating layers with different refractive indices,where the optical thickness of each layer corresponds to a quarter of the reflected wavelength.Owing to their vertical structure,DBR resonators can be integrated well with OLEDs.Additionally,they can effectively confine light to the cavity by reflecting it,thereby realizing laser oscillation.Figure 4 shows a DBR microcavity organic laser that observes electricallypumped quasi-continuous-wave lasing at an extremely low current density.Polariton lasing originates from the leakage of coherent photons from macroscopic exciton-polariton(EP)condensates via stimulated scattering,which is also known as the Bose-Einstein condensation(BEC)of EPs.Because population inversion is no longer required,polariton lasers are considered an alternative that may facilitate the development of practical electrically pumped organic lasers with much lower thresholds.As shown in Figure 5,strong coupling between excitons and cavity photons,referred to as room-temperature polariton lasing,is successfully observed in planar DBR cavities containing two new fluorene-based oligomers,BSFCz and BSTFCz.Within the WGM resonators,light is trapped owing to the total internal reflection at the interface,thereby realizing lasing oscillation.Section 2.3 summarizes the recent novel developments of electrically pumped organic lasers based on WGM resonators.WGM resonators typically possess high quality factors;however,their small size renders their fabrication and integration difficult.Figure 6 shows the realization of large microdisk arrays based on organic single crystals with the observation of WGM lasing from these microresonators. Conclusions and Prospects This study focuses on electrically pumped organic lasers.Based on different optical resonators,we summarize the recent novel developments of electrically pumped organic lasers from material selection to device optimization and then discuss the future development trends of electrically pumped organic lasers.Recent efforts toward electrically pumped organic lasers are important in the roadmap of organic lasers,which not only help us clarify the role of material synthesis,resonator design,device optimization,and photophysics in electrically pumped lasing but also provide insights into the fundamental knowledge,technologies,and strategies for solving the worldwide research problem of electrically pumped organic lasers.

High-sensitivity room-temperature multi-dimensional infrared (IR) detection is crucial for military and civilian purposes. Recently, the gapless electronic structures and unique optoelectrical properties have made the two-dimensional (2D) topological semimetals promising candidates for the realization of multifunctional optoelectronic devices. Here, we demonstrated the in-situ construction of high-performance 1T’-MoTe 2 /Ge Schottky junction device by inserting an ultrathin AlO x passivation layer. The good detection performance with an ultra-broadband detection wavelength range of up to 10.6 micron, an ultrafast response time of ~ 160 ns, and a large specific detectivity of over 10 9 Jones in mid-infrared (MIR) range surpasses that of most 2D materials-based IR sensors, approaching the performance of commercial IR photodiodes. The on-chip integrated device arrays with 64 functional detectors feature high-resolution imaging capability at room temperature. All these outstanding detection features have enabled the demonstration of position-sensitive detection applications. It demonstrates an exceptional position sensitivity of 14.9 mV/mm, an outstanding nonlinearity of 6.44%, and commendable trajectory tracking and optoelectronic demodulation capabilities. This study not only offers a promising route towards room-temperature MIR optoelectronic applications, but also demonstrates a great potential for application in optical sensing systems.

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The organic single crystal, due to its long-range ordered molecular arrangement, high quality, low defect state density, and excellent luminescent properties, plays an irreplaceable role in the field of optoelectronics and organic light-emitting diodes. By employing strategies for constructing organic single crystals, it is possible to significantly enhance the carrier mobility and stability of devices, leading to superior optoelectronic properties. In particular, in organic light-emitting diode (OLED) devices, the introduction of an organic single crystal luminescent layer can unlock the potential of luminescent materials, extend their operational lifetimes, and enable them to withstand higher current densities. Here, we have grown high fluorescence quantum yield (PLQY) blue-emitting 1,4-bis (2-methylstyryl) benzene (BMSB) molecules in single crystal form. The average mobility has been improved from non-existent in thin films to 0.188 cm2/(V center dot s) in crystal devices. Additionally, through the rational design of device structures and the enhancement of electrical properties, we have achieved a transition from non-functional thin film devices to stable blue-emitting crystal devices, achieving a current density of 853.60 mA/cm2.

Wearable epidermal electronics fabricated from MXene-based conductive hydrogels have attracted considerable interest because of their promising prospects in real-time health monitoring and human-computer interaction sensing. However, the development of a sustainable hydrogel with exceptional mechanical toughness, high conductivity, and self-adhesion is crucial to reliably capture signals through polymer network designs that establish robust interactions between MXene nanosheets and network substrates while minimizing electronic waste generated by discarded sensors. This study presents the fabrication of a sustainable conductive MXenebased dual-network hydrogel through skillful assembly of MXene nanosheets, beta-cyclodextrin with azobenzenemodified polyacrylic acid chains, and poly (vinyl alcohol) polymer networks. The hydrogel demonstrates exceptional mechanical properties (strength at breaking similar to 625 kPa, elongation at break similar to 630 %) attributed to the presence of numerous hydrogen bonds and host-guest interactions, along with superior electrical conductivity (23.65 S/cm) and self-adhesion. The hydrogel demonstrates exceptional sensitivity across a wide range of strains, enabling the detection of various human movements and achieving successful applications in handwriting recognition and sign language translation. Under acidic condition and UV irradiation, the disassembly of AZO and beta-CD as well as the untangling of PVA chains entanglement facilitate the release and recycling of MXene. This study presents a technological platform that holds promise for developing conductive hydrogels with enhanced sensing capabilities, catering to the requirements of stretchable electronic skin and intelligent robotic systems.

Efficient charge-carrier injection and transport in organic light-emitting devices (OLEDs) are essential to simultaneously achieving their high efficiency and long-term stability. However, the charge-transporting layers (CTLs) deposited by various vapor or solution processes are usually in amorphous forms, and their low charge-carrier mobilities, defect-induced high trap densities and inhomogeneous thickness with rough surface morphologies have been obstacles towards high-performance devices. Here, organic single-crystalline (SC) films were employed as the hole-transporting layers (HTLs) instead of the conventional amorphous films to fabricate highly efficient and stable OLEDs. The high-mobility and ultrasmooth morphology of the SC-HTLs facilitate superior interfacial characteristics of both HTL/electrode and HTL/emissive layer interfaces, resulting in a high Haacke’s figure of merit (FoM) of the ultrathin top electrode and low series-resistance joule-heat loss ratio of the SC-OLEDs. Moreover, the thick and compact SC-HTL can function as a barrier layer against moisture and oxygen permeation. As a result, the SC-OLEDs show much improved efficiency and stability compared to the OLEDs based on amorphous or polycrystalline HTLs, suggesting a new strategy to developing advanced OLEDs with high efficiency and high stability.