Vat photopolymerization (VPP) is a foundational additive manufacturing technology that fabricates objects layer by layer through photoinduced polymerization. Among its variants, mask projection vat photopolymerization (MP-VPP) has attracted considerable attention for combining high resolution and throughput with relatively low cost by utilizing dynamic masks. Despite these advantages, key process parameters such as exposure time and cure depth are often determined empirically, limiting reproducibility and scalability. To overcome this gap, we emphasize the importance of physics-based theoretical models that reveal the fundamental curing mechanisms, thereby supporting accurate process control and improved printing fidelity. This review introduces a unified spatiotemporal modeling framework for MP-VPP, grounded in first-principles physics and progressively incorporating temporal and spatial effects. Existing models are systematically categorized into two domains: (i) temporal-determination models, which describe curing kinetics, energy accumulation, and depth growth, and (ii) spatial-determination models, which address light propagation, optical interactions, and in-plane curing fidelity. For each category, recent advances are synthesized and their implications for optimization are discussed. The review concludes by outlining emerging challenges and research opportunities. By integrating temporal and spatial perspectives, this work strengthens the theoretical foundation of MP-VPP and facilitates its development toward more precise, reliable, and efficient manufacturing.

While main chain-main chain and side chain-side chain interactions are known to maintain protein architectures, the role of main chain-side chain interactions remains largely unexplored. Among various amino acid side chains, uncharged polar ones may uniquely modulate molecular conformations through directional hydrogen bonding (H-bonding) with the main chain. Using 15 minimalistic amphiphilic peptides, we demonstrate that intrastrand H-bonding between C-terminal uncharged polar side chains and the main chain dictates conformational preferences. Specifically, serine and threonine side chains significantly alter single-strand conformations, thereby reprogramming interstrand H-bonding modes in β-sheet assembly and generating distinct right-handed supramolecular chirality. This study elucidates how polar side chain-backbone H-bonding controls chirality and provides a rational design strategy for engineering peptide nanofibrils with rare right-handed chirality.

The rapid growth of wearable electronics demands power sources that are not only flexible and durable but also inherently safe. Conventional lithium-ion batteries pose safety risks due to toxic and flammable electrolytes. Aqueous metal-ion batteries offer a promising alternative, yet their application remains limited by poor mechanical compliance, leading to interfacial instability and electrolyte leakage. Here, we report a bionic self-assembly strategy for aqueous zinc-ion batteries using a lipopeptide electrolyte additive named C16K, enabling bulk self-assembly into supramolecular nanohelices to accelerate ion transport and interfacial organization into a dynamic bilayer for interphase regulation. This dual-function synergistically suppresses the formation of Zn dendrites or side reactions, enabling stable Zn plating/stripping. This achieves an ultralong cycling stability and ultrahigh cumulative plating capacity along with a high coulombic efficiency. Therefore, the synergistic reinforcement endows the pouch cell to deliver a high initial capacity, allowing to power electronics in a safe manner. In a following manner, a scorpion tail-inspired bionic flexible battery structure is designed to deliver sustainable energy outputs across various mechanical states using the reinforced systems, effectively powering the wearable multimodal sensors. Our results present a self-assembly strategy using a lipopeptide additive to synergistically reinforce the ions transport and interfacial stability, coordination with a bionic structural design, potentially offering a bioinspired routine for high-performance flexible batteries for wearable electronics.

Amino acid non-centrosymmetric self-assemblies, possessing inherent polarization as well as biocompatibility, can be employed as bioinspired alternatives for the development of implantable piezoelectric bioelectronics. This could enable the harvesting of biomechanical energy for in situ in vivo monitoring and avoid the need for secondary surgeries, potentially overcoming the trade-off between high-efficiency sensing and the biosafety limitations of traditional inorganic or polymeric piezoelectric counterparts. In this regard, the electromechanical coupling behaviors of the minimalistic metabolite self-assemblies are reported. Experimental tests reveal that compared to other natural amino acid crystals, threonine (T) crystals exhibit a high Young’s modulus of up to approximately 80 GPa by forming a denser three-dimensional hydrogen-bonding network, with each molecule interacting with seven adjacent ones. Computational analysis reveals that side-chain entities dramatically affect crystal packing, with polar hydroxyl moieties accounting for the distinct piezoelectric features underlying the macroscopic performance. This highlights the potential of exploiting T crystals to develop biodegradable piezoelectric bioelectronics that exhibit highly sensitive linear responses for tactile sensing and post-implantation in vivo motion monitoring. This study demonstrates the feasibility of exploiting minimalistic metabolite self-assemblies for piezoelectric bioelectronics in bio-machine interface and biomedical engineering applications.

Constructing stable and efficient bifunctional electrocatalysts is of great importance for green H-2 production via overall water splitting. This study prepares a heterostructure of Co2P and NiFe layered hydroxide (LDH) starting from a metal-organic framework (MOF) precursor. The Co2P nanoarrays derived from MOF are directly grown on Ni foam, ensuring high electrical conductivity and providing abundant surface active sites. Meanwhile, the synergistic coupling between heterogeneous structures significantly optimizes the charge transfer process. Therefore, when evaluated in alkaline electrolyte, the resulting Co2P@NiFe LDH-100 demonstrates promising electrocatalytic activity toward oxygen evolution reaction (OER, eta(100) = 230 mV) and hydrogen evolution reaction (HER, eta(10) = 88 mV). Moreover, an overall water splitting cell configured with Co2P@NiFe LDH electrocatalyst displays a low device voltage of 1.594 V to drive 10 mA cm(-2), and operates stably over 100 h. This study demonstrates a feasible route for designing efficient and low-cost bifunctional catalysts for water splitting applications.

Transition metal sulfides (TMSs) exhibit abundant active centers and cooperative redox activity, making them promising electrocatalysts for water splitting. Nevertheless, the practical implementation of TMSs is constrained by insufficient electrical conductivity and kinetically sluggish reactions. In this study, a Mott-Schottky heterojunction enriched with sulfur vacancies (NiCo@C/NiCoSv) is successfully synthesized on nickel foam (NF) via partial sulfidation of bimetallic nickel cobalt metal-organic framework (NiCo-MOF), followed by H2/Ar reduction. Mott-Schottky heterojunction-induced built-in electric field effectively accelerates charge transfer. Incorporating sulfur vacancies into electrode materials tailors electronic structure, which leads to markedly enhanced electrical conductivity while promoting electron/ion transfer kinetics. As a result, the resulting NiCo@C/NiCoSv achieves exceptional bifunctional activity in 1 M KOH, requiring overpotentials of only 260 mV for oxygen evolution reaction (OER) and 148 mV for hydrogen evolution reaction (HER) to reach 100 mA cm-2. The electrolytic cell using NiCo@C/NiCoSv as the anode and cathode only requires 1.48 V to output 10 mA cm-2, outperforming benchmark commercial electrodes. This work proposes a practical strategy for significantly improving the efficiency of overall water splitting of electrocatalysts by coupling heterojunction and vacancy engineering.

Compared with state-of-the-art polymeric counterparts, proteinic self-assemblies may bridge the gap between device performances and biocompatibility/biodegradability requirement, showing promising potentials in implantable bioelectronic scenarios. Nevertheless, stochastic behaviors due to lack of structural design severely restrict the reliability of proteinic sensors, along with hindering their miniaturization for in vivo applications. Herein, proteinic hydrogelation-based structured implantable sensors of intrinsic biodegradability with enhanced stability and sensing behaviours are engineered. Upon enzymatic crosslinking, the bio-hydrogels can boost mechanical elasticity and lead to minimal swelling side-effects for bioelectronics. Followingly, an interlocking sawtooth structure is designed to convert external loading into tensile strain, based on which a miniaturized implantable tactile sensor of high-performances is developed, showing an ultrahigh sensitivity integrated with fast dynamic responses, high resolutions towards varied amplitudes, frequencies and types, as well as reliable repeatability and intrinsic biodegradability. Our findings exemplify the feasibility of developing bio-hydrogelated structured sensors as biodegradable bioelectronics

Bouligand architectures, renowned for the helicoidal plywood morphologies composed of bio-building blocks in exoskeletons, exhibit exceptional and tunable mechanical rigidity while maintaining lightweight feature. Herein, inspired from nature, supramolecular Bouligand architectures are developed through hierarchical arraying of short peptides self-assemblies using a photocurable 3D printing strategy. The ordered helical arrangement of the peptide self-assemblies gives rise to an anisotropic gelled network. Especially, the behaviors can be programmatically modulated by controlling the self-assembly and printing parameters, allowing the bionic architectures deliver enhanced mechanical robustness and amplified piezoelectric responses along with possessing intrinsic cytocompatibility and tunable biodegradability. This exhibits sustainable electromechanical coupling responses to engineer bioelectronics for in vitro and in vivo applications. This study exemplifies a versatile approach for constructing bionic hierarchical architectures via peptides self-assembly, and establishes a promising framework for designing bio-entities of programmable and amplified properties applicable in bio-machine interfacing and biomedical engineering fields.

Abstract Bouligand-type helical structures in nature offer exceptional mechanical properties, inspiring efforts in biomimetic material design. However, existing strategies based on synthetic polymers face limitations such as poor biocompatibility and complex processing. Short peptides, with their inherent biocompatibility and ability to self-assemble into ordered nanofibers via non-covalent interactions, provide a promising alternative. This work explores a bioinspired strategy to construct Bouligand-like spiral arrays using self-assembling short peptides. A photo-curable peptide-based bio-ink is developed, and external electric fields are employed during printing to guide nanofiber alignment. This approach enables the fabrication of hierarchical structures with tunable anisotropy and mechanical performance, offering a new pathway for functional biomimetic materials.

Bioinspired supramolecular architectonics is attracting increasing interest due to their flexible organization and multifunctionality. However, state-of-the-art bioinspired architectonics generally take place in solvent-based circumstance, thus leading to achieving precise control over the self-assembly remains challenging. Moreover, the intrinsic difficulty of ordering the bio-organic self-assemblies into stable large-scale arrays in the liquid environment for engineering devices severely restricts their extensive applications. Herein, a gaseous organization strategy is proposed with the physical vapor deposition (PVD) technology, allowing the bio-organic monomers not only self-assemble into architectures well-established from the solvent-based approaches but morphologies distinct from those delivered from the liquid cases. Specifically, 9-fluorenylmethyloxycarbonyl-phenylalanine-phenylalanine (Fmoc-FF) self-assembles into spheres with tailored dimensions in the gaseous environment rather than conventional nanofibers, due to the distinct organization mechanisms. Arraying of the spherical architectures can integrate their behaviors, thus endorsing the bio-organic film the ability of programmable optoelectronic properties, which can be employed to design P-N heterojunction-based bio-photocapacitors for non-invasive and nongenetic neurostimulations. The findings demonstrate that the gaseous strategy may offer an alternative approach to achieve unprecedented bio-organic superstructures, and allow ordering into large-scale arrays for behavior integration, potentially paving the avenue of developing supramolecular devices and promoting the practical applications of bio-organic architectonics.

The formation of dendrites associated with corrosion reactions undermines the cycling stability of aqueous zinc‐ion batteries (AZBs). Despite extensive efforts, conventional strategies, e.g., electrolyte modification, and artificial protection layers, often suffer from low stability. Inspired by cell membranes, a series of phospholipid analogues C n P m C is designed which can spontaneously adsorb onto the Zn electrode to form a bimolecular protective layer. By tuning the head length or the tail length of the lipid analogues, the nanostructures of the lipid layer can be modified in terms of coverage and thickness, affecting the electrochemical behavior of the electrode. The most optimal electrochemical behavior is found for the adsorption of C 12 P 2 C at a concentration of 1 mM. The bilayer formed by C 12 P 2 C is denser and more stable than those formed by other lipid analogues. The lipid bilayer facilitated the balance of Zn plating/striping, thereby effectively limiting the growth of dendrites and side reactions, further enhancing the reversibility of zinc‐based aqueous batteries. In symmetric battery experiments, C 12 P 2 C can exceed 3600 h under 1 mA cm −2 and 1 mAh cm −2 test conditions. Thus, this study not only demonstrates a bio‐friendly electrode protective material but also provides constructive suggestions on the molecular design of electrode protection material.

As the largest organ in the human body, the skin plays a crucial role in protecting tissues from external threats. Damage in the skin can not only lead to bleeding and increase the risk of infection and inflammation but also result in tissue necrosis and scar formations. Therefore, wound dressings of high efficiency and intrinsic biocompatibility are essential for defending the wound sites and promoting healing. However, the state-of-the-art wound dressings have intrinsic shortcomings in curing, which would exudate due to limited water absorption capacity and the adhesion side effect, which may cause secondary damages. There remains a gap in the availability of wound dressings that simultaneously integrate antibacterial, self-healing, biodegradable, and temperature-sensitive properties. Herein, a bioinspired supramolecular hydrogel-based wound dressing composed of a KYD (KYDYKYDYKK) self-assembly peptide-agar double-network is developed with the assistance of 3D printing. The reversible self-assembling dynamics of the KYD along with the existence of lysine residues endow the double-networks with the ability of self-healing and antibacterial properties, while the introduction of agar allows the bioinspired system to be temperature sensitive. In addition, the grid size of the bioinspired dressing is light-stimulated and adaptable, allowing for real-time control of air permeability. Combined with intrinsic biodegradability, the multifunctional supramolecular wound dressing enables sustainable drug releases. Consequently, the programmability of strength, flexibility, and performances in this design ensures customizability in a variety of wound conditions of the bioinspired supramolecular wound dressing, thus showing promising potential in enhancing clinical wound management and improving patient lifecare.

Hypothesis Bioengineered monoclonal antibodies (mAbs) have gained significant recognition as medical therapies. However, during processing, storage and use, mAbs are susceptible to interfacial adsorption and desorption, leading to structural deformation and aggregation, and undermining their bioactivity. To suppress antibody surface adsorption, nonionic surfactants are commonly used in formulation. But how surface hydrophobicity affects the adsorption and desorption of mAbs and nonionic surfactants individually and as a mixture remains inconclusive. Experiments The rapid tuning of the siliconized surface from hydrophobic to hydrophilic was controlled by the UV oxidation time of a self-assembled trimethoxy(7-octen-1-yl)silane (TMOS) monolayer. Spectroscopic ellipsometry and neutron reflection were used to determine the dynamic adsorption and structural changes of the co-adsorbed mAb (COE-3) and the commercial nonionic surfactant PS80, which is composed primarily of polyoxyethylene-sorbitan monooleate with an average molecular weight of about 1310 g/mol. Findings COE-3 adsorption on both TMOS or UV-TMOS surface was irreversible. However, nonionic surfactant PS80 could partially remove pre-adsorbed COE-3 from these surfaces, forming a co-adsorption layer. Interestingly, while the hydrophobic TMOS surface prevented mAb adsorption when pre-treated with PS80, the amphiphilic UV-TMOS did not. Furthermore, when COE-3 and PS80 were injected as a mixture, PS80 formed a preventative layer on both surfaces against COE-3 adsorption. These results highlight the significance of surface hydrophobicity in controlling mAb adsorption in the presence of nonionic surfactants.

Crystallized peptide assemblies have demonstrated useful physicochemical and electromechanical features due to the highly ordered supramolecular packing driven by efficient and extensive non-covalent interactions. However, the structural polymorphism of the bioinspired self-assemblies poses challenges for their rational design and scale production as sustainable, eco-friendly, and tailorable materials for technology applications. Here, it is demonstrated that peptide polymorphic crystallization is a hierarchical process, evolving from initially flexible, twisted nanofibrils bundling to form ribbons, then ripening to robust, plate-like crystals composed of superhelices, as observed using high-resolution microscopy and crystallography supported by molecular dynamics simulations and quantum mechanical calculations. The hierarchical process accounts for the known morphological diversity of peptide crystals and provides a mechanism of controllably restricting the assembly to create only specific supramolecular structures as demanded. Especially, the superhelical organization enables high-efficiency energy transformation, resulting in tremendous photoluminescent, optical waveguiding, and electromechanical energy-harvesting potential. These findings endorse the feasibility of connecting the bioinspired flexible aggregations and robust crystallizations.

Aqueous zinc-ion batteries (AZIBs) are appealing devices for cost-effective and environmentally sustainable energy storage. However, irreversible issues such as dendrites, corrosion and hydrogen evolution reaction at the anode threaten to hamper their widespread deployment. Herein, we propose synergic self-assembly and arraying to form ordered bionic supramolecular pillar-like architectures (BSPAs) on the Zn anode through physical vapor deposition (PVD). With the combination of physicochemical and electrochemical characterizations, we demonstrate that the BSPAs exhibit a superhydrophobic feature with an ultrahigh contact angle up to 160.4 degrees, and provide ordered zincophilic channels with a low activation energy of 34.91 kJ mol(-1) due to the presence of well-organized electronegative N entities in the assemblies. This allows desolvation of Zn2+ and promotes fast transportation and uniform deposition of Zn without dendrites. Consequently, the BSPAs@Zn-based symmetric cells achieve a long cycling stability of over 1000 h at 1 mA cm(-2) and 1 mAh cm(-2), and the BSPAs@Zn||MnO2 full cells exhibit an improved rechargeability up to 600 cycles with 50.0 % capacity retention at a high current density of 5.0 A g(-1). This work paves the avenue of developing large-scale molecular self-assembly in reducing water adsorption and regulating the Zn deposition, potentially providing an efficient approach to stabilize the AZIB anode.

Inspired by the stimulation of biological systems, cyclic dipeptides self-assemble through the synergistic driving of various non-covalent interactions, such as hydrogen bonding and pi- pi stacking, to form functional materials with long-range ordered nanostructures, whose excellent physicochemical properties, such as unique photo-responsive properties and biocompatibility, have a wide range of applications in the fields of bio-photovoltaics and energy harvesting. In this paper, we focus on the structure-mechanism-function linkage of cyclic dipeptide self-assembly, and systematically illustrate its transition from basic research of molecular design to application. At the level of self-assembly mechanism, the entropy-driven crystallization dynamics is revealed, and the intermolecular forces and stacking arrangement are confirmed by crystallographic characterization techniques; at the level of functionality, the multi-dimensional applications of cyclic dipeptides as low-loss organic optical waveguide materials, piezoelectric sensors, and anti-bacterial and anticancer materials are analyzed. Through the establishment of non-covalent interaction network-microstructure-macroscopic performance constitutive model, we will point out the technical route for the development of biodegradable bioelectronic devices and intelligent drug delivery systems, and promote the cyclic dipeptide materials from basic research to the leapfrog development of precision medicine and flexible electronics industry.

Despite numerous reports devoted to chirality inversion during the self-assembly of single chiral components, chirality inversion in the coassembly of two or more chiral components remains largely unexplored. Here we report the supramolecular chirality inversion via the coassembly of the two different stereoisomers of a minimalistic amphiphilic I3K sequence with like-handedness in their self-sorting assembly. The coassembled nanofibrils exhibit noticeable helix inversion in a wide range of mixing ratios, compared to individual peptide nanofibrils. Theoretical simulations reveal that to facilitate the interstrand H-bonding between isomeric β-strands within a mixed β-sheet, those with a homochiral backbone will undergo chirality inversion due to their structural flexibility. The inverted strands with two heterogeneous interfaces within the sheet typically display larger twisting degrees and are responsible for inducing helix inversion of the sheet and final β-sheet nanofibrils, and thus, helix inversion of the final nanofibrils can be regulated by tuning the ratio of the two components. This study lays a foundation for manipulating the suprastructure chirality of peptide bionanomaterials through coassembly.

Bioinspired piezoelectricity is extensively explored for diverse bio-machine interface and biomedical engineering applications. Nevertheless, state-of-the-art bio-piezoelectricity mainly focuses on crystallization. Yet, crystalized structures exhibit several shortcomings, including limited biocompatibility or biodegradability along with intrinsic non-stretchability. Herein, peptides fibrillization is reported to present inherent bio-piezoelectricity. Upon forming double-network framework with silk fibroin, fibrous peptide piezogels of innate biocompatibility and biodegradability are achieved, showing a programmable piezoelectricity. In particular, the bioinspired supramolecular piezogel can linearly respond to external compression and stretching in large force regions, extensively expanding the application potential bio-piezoelectricity. Upon designing a "W"-shaped structural conformation, a peptide fibrous piezogel-based piezoelectric sensor is shown to be used for detection of limb movements and subcutaneous implantation of the bioinspired piezoelectric electronics, realizing in situ and real-time monitoring of stimuli responses. The findings suggest the promising potential of peptide fibrillization-based bio-piezoelectricity for diverse bio-machine interface and biomedical engineering applications.

Nitrogen dioxide (NO2) is an important contaminant that poses a severe threat to environmental sustainability. Traditional inorganic NO2 gas detectors are generally used under harsh operating conditions and employ environmentally unfriendly resources, thus preventing widespread practical applications. Herein, self-assembled peptide microtubes (SPMTs) are combined with SnO2 nanoparticles (NPs) to develop a bioinspired NO2 gas sensor. The sensor incorporated with SPMTs exhibits a lower resistance and a stronger response under visible light irradiation. Under exposure to 4.7-mW/cm2 white light irradiation, the device exhibits a response of 412 and a resistance of only 97 MΩ, contrast to 318 and 340 MΩ for the bare SnO2-based counterpart under the same test conditions. This work exemplifies the feasibility of using bioinspired approach employing peptides self-assembly strategy to engineer comprehensive pollution detectors, potentially enabling development in the environmentally friendly sensing field.

There is a growing demand for sustainable and safe materials in developing technological systems and devices, including those that enhance Raman scattering. Organic (bio) materials based on simple peptides are one class of such materials. This study investigates self-assembled semiconducting peptides as metal-free substrates for surface-enhanced Raman scattering. Our results reveal significant variations in Raman enhancement factors, spanning up to 2 orders of magnitude. We examined specific Raman enhancement selection rules related to the energy levels and structural configurations of the probe molecules. The effectiveness of these rules underscores the importance of strong molecule-peptide coupling and efficient charge transfer for achieving optimal Raman enhancement factors. These insights offer a foundational understanding of peptide-molecule interactions and the underlying chemical mechanisms driving Raman enhancement, highlighting the potential of organic semiconductor-based materials as highly effective platforms for enhancing Raman scattering in chemical sensing applications.