Twist imparts nonlinear shear stress and induces entropy changes in materials, forming the fundamental basis of twistocaloric cooling. This refrigerant-free and energy-efficient approach offers a promising alternative to conventional vapor-compression cooling systems. It provides distinct advantages, including low driving stress, considerable cooling power, and compatibility with flexible devices. Despite increasing efforts, a universal structure-performance relationship linking molecular design to device-level cooling behavior remains elusive. In this review, we summarize recent advances in twistocaloric cooling materials and devices, highlighting the growing demand for twist-based structures in thermal management. We focus on the molecular design and structural characteristics of representative twistocaloric materials, including shape memory alloys, entropy-elastic polymers, and semi-crystalline fibers, and compare their cooling capacities arising from twist-induced stress field and hierarchical molecular alignment. Strategies for enhancing cooling amplitude and coefficient of performance are also discussed alongside emerging device architectures that leverage nonlinear stress fields for high integration, low actuation force, and long cycle life. Further, we present the remaining challenges and further perspectives of the twistocaloric field, emphasizing pathways toward intelligent, mechanically robust, energy-efficient, and environmentally adaptable thermal management technologies.

Topical transdermal drug delivery strategies for psoriasis offer advantages including precise targeting, favorable safety, and enhanced patient compliance compared to systemic administration. However, a formidable challenge remains in achieving effective percutaneous penetration of therapeutics across the hyperkeratotic stratum corneum to elicit optimal therapeutic efficacy. In this study, we constructed a small-sized amorphous solid dispersion (S-SD) stabilized by zwitterionic hyperbranched polycarbonate (HP-CB) for transdermal delivery of baicalin (BAI) and psoriasis therapy. The BAI-loaded zwitterionic S-SD (SZ-SD@BAI) synergistically enhanced the solubility and permeability of BAI by over 102.5 times in pure water and 2.6 times respectively compared with free BAI. The ultra-small size of SZ-SD@BAI facilitates initial penetration through the stratum corneum, while its zwitterionic surface reduces electrostatic repulsion, minimizing non-specific interactions with biological macromolecules and disrupting lipid and keratin structures via a “fluidization” effect. Additionally, it combines with lipids to form “drug storage” and selectively extracts lipid components thereby achieving a continuous release to the deep epidermis and dermis. Furthermore, SZ-SD@BAI effectively suppressed lipopolysaccharide-induced abnormal proliferation of HaCaT cells and demonstrated potent antioxidant activity. In vivo tests confirmed that SZ-SD@BAI markedly reduced the area and severity index of psoriasis, improved immune dysregulation and oxidative stress, and exhibited favorable biocompatibility with low hemolysis. Based on these advantages, SZ-SD@BAI was further developed as a cream preparation and showed enhanced efficacy compared to the clinical reference drug tacrolimus. This research presents an innovative and highly efficient transdermal formulation applying SZ-SD, which offers a promising foundation and delivery strategy for addressing psoriasis and various other skin disorders.

High-efficiency refrigeration materials with long cycle lifetimes are essential for reducing energy consumption in conventional cooling systems. Twistocaloric cooling, which harnesses nonlinear torsional stress, offers a promising pathway to enhanced cooling efficiency. However, a general design strategy for polymer-based twistocaloric materials that combine high efficiency and long cycle life remains elusive. Here, we report spider silk-inspired polybiurea elastomer fibers that exhibit exceptional mechanical properties and twistocaloric cooling performance. The material's architecture features nanoknot-like domains formed via multiple hydrogen bonds and π-π interactions in the hard segments, which knot together the soft segments to provide high mechanical stability and substantial entropy changes. The polybiurea fibers with nanoknot-like domains achieved an extraordinary combination of breaking strength of 316.5 MPa and toughness of 523.4 MJ m-3. This engineered deformable knotted structure enables a maximum cooling temperature drop of -17.1 K (by twisting and stretching), a maximum Carnot efficiency of 89.7%, and operational durability up to 120 000 mechanical fatigue life cycles. We further demonstrate two out-of-phase operated twistocaloric devices designed to recover input mechanical energy, thereby enhancing overall system efficiency. This work presents a robust materials strategy for advancing high-performance polymeric refrigeration materials and systems.

Natural spider silk achieves its exceptional performance through the synergy of rigid β-crystallite anchors and stretchable, energy-dissipating β-sheet domains. However, perfectly replicating this architecture in biomimetic systems remains a significant challenge. Here, we report the development of super-tough artificial silk fibers utilizing a hybrid covalently anchored network (CGN) architecture based on bioinspired glue-like nanoparticles (GNPs). By integrating these GNP cross-links into a stable covalent network, we created a system where adsorbed polymer chains on the GNPs form dynamic loops with substantial hidden lengths. Upon stretching, these loops unfold and dissipate massive energy via the sacrificial rupture of interfacial bonds, mimicking natural β-sheet domains. Crucially, adjusting GNP cross-link size and interfacial binding strength enables precise tuning of the fiber's mechanical balance. Furthermore, the stable covalent skeleton serves as a topological anchor, imposing entropic penalties on chain desorption. This constraint suppresses polymer detachment from the GNP surfaces, compelling chains to undergo stress-induced orientation and assemble into highly aligned nanofibrils. The resulting fibers achieve a tensile strength of 1.25 GPa and a toughness of 306 MJ m-3, successfully reproducing the strength-toughness synergy of native silk. This approach offers a scalable pathway for engineering high-performance fibers for applications in artificial muscles and advanced actuators.

INTRODUCTION:Effective pulmonary vaccination remains limited by the pulmonary surfactant (PS) barrier and inefficient intracellular delivery of vaccine cargo to alveolar antigen-presenting cells, particularly alveolar macrophages. Inspired by the natural compatibility of alveolar macrophage-derived vesicles with the alveolar environment, we developed biomimetic alveolar macrophage membrane vesicles (AMVs) as a mucosal nanocarrier platform. OBJECTIVES:This study aimed to develop a nanovaccine platform that addresses key extracellular and intracellular barriers in the lung and to evaluate its immunogenicity and protective efficacy in multiple respiratory pathogen models. METHODS:AMVs were engineered to improve performance in the PS environment and to achieve preferential uptake by alveolar macrophages. An Antigen Capture and Cytosolic Delivery System (ACCDS) was incorporated, comprising: (1) an engineered surfactant protein A domain for broad pathogen binding; (2) a pH-responsive listeriolysin O module designed to facilitate endo/lysosomal escape and enhance cytosolic access of cargo; and (3) encapsulated Poly(I:C) to activate TLR3 and support RIG-I/MDA5-associated signaling. RESULTS:AMV-ACCDS-Poly(I:C) showed improved delivery performance in the PS-associated environment and preferential uptake by alveolar macrophages compared with synthetic nanoparticles and a commercial transfection reagent. Dual innate activation was associated with stronger IFN-β and IL-18 responses than those induced by the tested control formulations. The platform promoted the local establishment and/or differentiation of lung-resident memory-like CD8+ T cells and was accompanied by IL-18-associated metabolic remodeling. In prime-boost studies, it conferred complete protection in lethal influenza and pseudorabies virus challenge models and reduced pulmonary burden in a Mycoplasma infection model. CONCLUSION:AMV-ACCDS-Poly(I:C) provides a biomimetic strategy to address key barriers in pulmonary vaccination and supports the potential of membrane-based mucosal vaccine systems for protection against respiratory pathogens.

Electrothermal polymer artificial muscles are increasingly popular in soft robotics due to their high load‐to‐weight ratio and cost‐effectiveness. However, current control strategies for these actuators mostly rely on traditional proportional integral derivative (PID) control or single‐dimensional closed‐loop control. These methods can mitigate the adverse effects of the inherent hysteresis, nonlinearity, and temperature–force angle coupling of these actuators somewhat, but fail to effectively meet the precision requirements of specialized applications. To address these challenges, a temperature self‐sensing‐driven hierarchical closed‐loop fractional‐order proportional integral derivative (FOPID) control scheme is designed. It leverages nickel wire's resistance‐temperature characteristics for real‐time temperature self‐sensing, eliminating the need for external sensors; its hierarchical structure prioritizes temperature control followed by angle regulation to mitigate coupling effects; and the FOPID controller outperforms traditional PID with smaller overshoot and faster convergence to manage nonlinearity. Based on this control scheme, an artificial muscle is fabricated using polyethylene and silver‐plated nylon (PE@SPN). To enhance deformation and output force, single PE@SPN fibers are combined in series–parallel to form composite artificial muscles. A rehabilitation manipulator is developed based on these composite artificial muscles, with a closed‐loop control algorithm implemented via temperature self‐sensing and FOPID as the core control strategy, demonstrating the engineering application value of PE@SPN artificial muscles.

High-strength and tough fibers are essential in biological systems, such as ligaments and tendons, where they preserve tissue integrity under mechanical stress. Spider silk uniquely combines exceptional strength and toughness, arising through the hierarchical self-assembly of spidroin, while also offering excellent biocompatibility and inherent biodegradability, making it an ideal candidate for biomedical applications. Here, we demonstrate that rearranging spidroin peptide chains into ultrafine nanofibrils yields engineered natural spider silk fibers with markedly enhanced both mechanical and functional performance, achieving a breaking strength of 2.0 GPa, toughness of 480 MJ m-3, and actuation stress of 92.6 MPa. Importantly, the contractile actuation enables these fibers to function as a self-adapting surgical suture: beyond passive wound closure, the fibers actively generate postoperative stress, improving tissue approximation and promoting repair. This work establishes a generalizable strategy for engineering natural fibers with integrated mechanical robustness, actuation, and biomedical utility, opening new avenues for intelligent biomaterials design.

The cellular uptake efficiency and endocytic mechanism of nanocarriers are highly correlated with their size. Compared to inorganic nanoparticles, the acquisition of uniform sub-10 nm polymeric nanoparticles remains a challenge. Herein, uniform sub-10 nm crosslinked polymeric nanoparticles loaded with berberine (s-PPP-MC@B NPs) were successfully prepared via a combination of self-emulsifying dispersion and ultraviolet cross-linking technology. This approach effectively addresses the issue of nanoparticles size enlargement during selfemulsification in an acidic environment. Furthermore, the cross-linked shell enables the s-PPP-MC@B NPs to maintain sub-10 nm in acidic environments and to release berberine (BBR) in a sustained manner under neutral conditions in vivo. The s-PPP-MC@B NPs can efficiently achieve cellular internalization without the need for complex ligands. In combination with the permeation enhancer SNAC, they act synergistically to enhance the transcellular transport efficiency and significantly improve mucus penetration. Results show that blood glucose levels can be effectively reduced for over 21 h and that the BBR bioavailability is increased by 2.6-fold. Overall, this study proposes a simple, feasible method for preparing uniform sub-10 nm polymeric nanoparticles for use in drug delivery systems.

Currently, the development of artificial muscles that simultaneously possess high sensitivity, high linearity, and self-sensing capabilities remains a significant challenge. Inspired by the spider’s slit organ, a novel carbon nanotube/liquid crystal elastomer (CNTs/LCE) artificial muscle has been developed. This structure integrates a crack-based sensing unit, a helical deformation mechanism, and self-sensing functionality. A monolithic architecture featuring a helical crack sensor was constructed, which maintains high sensitivity while achieving a large deformation range. In this configuration, the helical structure serves to "kill two birds with one stone": it acts as a sensor that significantly enhances the strain capability, while also functioning as a twisted helical artificial muscle. Furthermore, the introduced crack structure markedly improves sensing sensitivity. When combined with a porous structure that enhances deformability, and utilizing the helical geometry to further amplify the deformation amplitude (up to 110

Hydrogel fibers are promising candidates for artificial tissues, yet achieving high mechanical robustness with high water content remains challenging. Here, we report a deformation-driven strategy that converts strain localization into a controllable pathway for necking created in a nano-assembly in single-component hydrogel fibers. By integrating wet spinning and confinement-assisted drying to form an oriented densified core-sheath structure, followed by programmed necking and salting-out treatment, super strong and tough poly(vinyl alcohol) hydrogel fibers are fabricated. This structure enables spatially confined necking to generate amplified local strain, thereby accelerating chain disentanglement and orientation and promoting nanofibrillar assembly and refined nanocrystalline organization. The resulting fibers exhibit exceptional mechanical performance, reaching a maximum tensile strength of 122.5 MPa, a maximum toughness of 350.4 MJ m-3, and a high water content of 67.9%, comparing favorably with previously reported hydrogel fibers. Moreover, the fibers maintain their shape, sustained mechanical performance, and long cyclic life under simulated body-fluid conditions for 7 days, demonstrating promising potential for artificial ligament application. This study provides a scalable route to high-performance hydrogel fibers and offers new insights into harnessing deformation-enabled structural programming for soft yet robust tissue-mimetic materials.

Inspired by the β-sheet nanocrystals in natural spider silk, we develop a high-damping polycrystalline-phase liquid crystal elastomer (LCE) fiber enabled by a semi-interpenetrating network. Continuous large-scale fabrication of this crosslinked system is realized using a unique channel-confinement strategy. By innovatively designing the end-group molecular structures of linear polymers, we precisely regulate the liquid-crystal phases within the semi-interpenetrating network fibers. Four distinct liquid-crystal phases are constructed, mimicking the β-sheet nanocrystals of spider silk to enable efficient energy dissipation. The resulting fibers exhibit a high elastic modulus of 47.6 MPa, outstanding toughness of 60.4 MJ m-3, a high dissipation coefficient of 88.6%, an ultra-broad damping temperature window, a wide damping frequency range, and a strong actuation stress. When woven into damping nets for impact buffering, the nets exhibit a tunable memory recovery time and an exceptionally low dynamic rebound ratio of 5.9%, enabling efficient impact-energy adsorption and secure capture. Overall, this work overcomes the long-standing trade-off among mechanical, actuation performance, and damping capacity of LCEs, and provides a universal strategy for elastomer-based damper design and precise liquid crystal phase control, opening new opportunities for applications in elastomer dampers, artificial muscles, and soft robotic systems.

Self-oscillating actuators that can achieve autonomous motions are highly desired in autonomous soft robotics and intelligent devices. Moreover, oscillators driven by multi-stimuli have attracted considerable interest and have potential applications in multiple complex environmental systems. However, most actuation systems require manual control of switches, and film-based twisting/untwisting oscillation and length stretching/contraction oscillation have not been realized. Here, we fabricated a helical nanofiber composite film and achieved twisting/untwisting oscillation, bending oscillation, and elongation/contraction oscillation under heat, light, and moisture stimuli. Moreover, the oscillator can realize continuous mechanical work under different loads as well as continuous electrical output. This study not only provides the twisting oscillation and twisting motion mechanism but also presents a versatile strategy to fabricate hydrogel-based bilayer hierarchical porous nanofiber composite film twisting oscillators. This actuation system with a twisting self-oscillation load capacity and a multi-stimuli response will be used for autonomous smart devices, autonomous energy conversion, and multi-scenario applications.

A highly atom- and step-economic palladium-catalyzed sequential hydrofunctionalization of skipped enynes with phenolic compounds has been developed. This approach provided an efficient method to construct chromans in moderate to good yields with high regio-, chemo-, and stereoselectivities, exhibiting good functional group compatibility and gram scalability. Preliminary mechanistic studies indicated that the single palladium catalyst is capable of effectively facilitating both the intermolecular hydroarylation and intramolecular hydroaryloxylation process.

Developing high-performance bio-based fibres is highly desirable for improving the sustainability of materials. Cellulose is one of the most abundant bio-derived feedstocks to fabricate such materials. However, the fabrication of high-strength macro cellulose fibres is challenging due to the difficulty in obtaining ordered packing of cellulose molecular chains and nanocrystals in the macro-fibres. Here we develop a draw spinning/de-acetylation method to prepare cellulose fibres with highly ordered molecular packing that incorporates high strength in the obtained fibres. Specifically, a fibre draw spun from well-dispersed cellulose triacetate solution was de-acetylated to generate cellulose fibres, which were then twisted to spirally align the molecular chains. The resulting fibres exhibited mechanical strength of 3.08 GPa and toughness of 215.1 MJ m-3, much higher than existing fibre materials. This work paves the way to obtaining high-performance bio-based fibres.

The pursuit of biomimetic fibers with simultaneous high toughness and strength persists, despite their inherent trade-offs.However, for artificial spider silk based on gel fiber, it is still unclear for the molecular chain attributes related to the improvement of the strength and toughness. Here, a hydrogel fiber was prepared by mimicking the molecular structure of natural spider silk, and we delved into the molecular chain structure characteristics related to the strength, toughness and damping capacity of gel fiber, such as crosslinking density, molecular chain orientation and hydrogen bond interaction. The results indicate that a certain increase in crosslinking density and molecular chain orientation contributes to the enhancement of tensile strength, while the toughness and damping remain essentially unaltered. The thermal dissociation of hydrogen bond could enhance the toughness in a specific range, while the humidity destruction of hydrogen bond would reduce the toughness.Through well-regulation control of the weight ratio of polyacrylamide（PAM） to poly（acrylic acid）(PAA), the PAM@PAA gel fibers could reach maximum breaking strength of 1.02 GPa, maximum toughness of 149 MJ m -3 , and damping capacity of 95%.PAM@PAA gel fiber has demonstrated excellent wound healing performance and biocompatibility in vivo evaluation as a surgical suture, which indicates its potential in biomedical applications.

1,3-Dioleoyl-2-palmitoylglycerol (OPO) is crucial for infant nutrition; however, conventional immobilized lipase requires high-purity enzymes, which increases costs and limits industrial scalability. Herein, Rhizomucor miehei lipase (RML) was immobilized on surface-modified magnetic nanoparticles using cross-linked enzyme aggregates (CLEAs) technology to produce Fe3O4@SiO2@TPOAC@RML CLEAs. This approach combines the separation and immobilization of enzymes, allowing for the use of lower-purity lipase, which enhances its suitability for industrial-scale processes. The optimized Fe3O4@SiO2@TPOAC@RML CLEAs exhibited excellent thermal, pH, and storage stability. The performance of Fe3O4@SiO2@TPOAC@RML CLEAs was evaluated by catalyzing the synthesis of OPO through the enzymatic hydrolysis of glycerol tripalmitate (PPP) and oleic acid (OA). Under optimal conditions, the OPO content in products reached 63.33 ± 0.30%, highlighting the high efficiency of the enzymatic process. After eight reuse cycles, the Fe3O4@SiO2@TPOAC@RML CLEAs retained around 75% of their relative activity. Therefore, this strategy of lipase immobilization using CLEA technology, coupled with magnetic nanoparticles, offers a promising approach for OPO synthesis.

Although machine learning (ML) has been widely applied to drug solubility prediction, most existing models focus on single-solvent systems, and accurate prediction in complex micro-environments (mixed solvents) remains challenging. Herein, we report the first predictive framework that integrates mechanism-driven microscopic variables (molecular descriptors and Hansen solubility parameters) into three ML algorithms: artificial neural networks (ANN), support vector machines (SVM), and random forests (RF). Among them, RF achieved the best performance, with the coefficient of determination (R2) markedly improved from 0.830 to 0.988 when Hansen parameters were included as input features. Analysis of factor interactions revealed that solvent hydrogen-bonding capacity, polarity, mixing ratio, and temperature play key roles in modulating drug solubility, consistent with previous experimental studies. These results underscore the critical role of microscopic variables in capturing solubility behavior in mixed solvent systems. More broadly, this work demonstrates that integrating mechanism-driven descriptors with data-driven ML models offers a powerful and generalizable strategy for accurately predicting drug solubility in complex micro-environments.

ConspectusLiquid crystal elastomer fibers (LCEFs) are reversible artificial muscles capable of stimuli-responsive functions, making them promising competitors for ideal soft actuators. These remarkable actuation properties depend strongly on their mechanical properties, such as elastic modulus and breaking stress. It is necessary to strengthen the LCEF muscles to meet the demands of advanced applications. However, despite the significant progress in LCEFs, there is currently no such Account systematically summarizing and analyzing the strategies adopted for enhancing their mechanical and actuation properties. The intuitive variations among the different enhancement strategies further call for investigations into how to choose the most suitable ones based on specific situations. In this Account, for the first time, we systematically summarize existing approaches to strengthening LCEF-based artificial muscles, contributing to the development of more robust and smarter fibrous artificial muscles.In the first section, we focus on the latest and most valuable progress on strengthening LCEF-based artificial muscles, highlighting the need for a comprehensive summary of the various approaches utilized. The mechanical properties of LCEFs can be tailored through molecular design, physical interactions, and fiber integration. The adjustment of hard/soft segment features, the introduction of additional microstructures, and the fiber integration provide opportunities to strengthen LCEF-based artificial muscles, which are discussed in the second section. Subsequently, we delve into the impact of various preparation methods on the performance of LCEFs, and LCEFs fabricated by different spinning and alignment techniques exhibited rather different mechanical and actuation properties. This has been adopted to engineer novel, stronger, and tailored fibrous artificial muscles, as described in the third section. Moreover, we show that the incorporation of rigid composite materials via coating and doping has emerged as a powerful strategy to strengthen LCEFs, such as core-shell structures. Such enhancements also introduce multifunctionality for LCE-based artificial muscles that can enrich the fiber structure and actuation mechanism, which are elucidated in the fourth section. Finally, we conclude this Account with a critical analysis of the challenges and prospects of LCE-based artificial muscles, hoping to pave the way for the construction of more powerful fibrous artificial muscles.

In nature, many animals protect themselves through deformation, discoloration, and infrared concealment to achieve multiple forms of camouflage. Camouflage fabrics designed for deserts and rainforests have vastly different requirements for color, breathability, and infrared emission. However, the development of corresponding smart fabrics remains a significant challenge. In this work, a novel dynamic-bond-controlled hygro-responsive hydrochromic wool fiber artificial muscle, inspired by the octopuses, has been developed, which used to construct a smart multi-camouflage fabric that integrates deformation, allochromasia, and infrared concealment. The obtained fabric exhibits a green color in humid environments (rainforests), with large pores for perspiration. In a dry environment (deserts), the fabric contracts and changes to akhaki color, while the reduction in pore size enhances infrared shielding. As the relative humidity increases from 20% to 100%, the average pore size of multi-camouflage smart fabric decreases by similar to 84%, minimizing the radiative temperature difference between 36 degrees C target. This results in a temperature reduction of 5.2 degrees C for the target. The hydrochromic artificial muscle is also employed to develop smart fabrics that mimic octopus-like behaviors. With its biocompatible, biodegradable, high thermal insulation, and comfortable wearability, the dynamic-bond-based multifunctional muscle fabric opens up additional possibilities for smart textiles, information technology, and artificial intelligence.

Polymeric materials research is increasingly directed toward biomimicry, exploring designs derived from nature's long evolutionary processes to enhance material properties and sustainability. Scientists have long recognized that spider silk, as a natural polymer, possesses exceptional physicochemical properties, including high tensile strength, superior toughness, good thermal conductivity, ultracontraction, and unique torsional rotation driving capabilities. These remarkable characteristics have inspired ongoing efforts to develop biomimetic spider silk materials, with the aim of replicating the natural structure of spider silk to create polymers with similar or even superior performance. This article aims to explore the synthesis methods of high-performance biomimetic polymer materials, such as artificial spider silk, and their advanced applications across various fields. The review will discuss recent advances in the synthesis of novel artificial spider silk materials, focusing on polymer molecular design, the construction of secondary cross-linked networks, micro-nano assembly structure, and the development of innovative spinning techniques, as well as the potential of artificial spider silk in biomedical and flexible smart wearable applications.