It is highly desirable, although very challenging, to develop self‐healable materials exhibiting both high efficiency in self‐healing and excellent mechanical properties at ambient conditions. Herein, a novel Cu(II)–dimethylglyoxime–urethane‐complex‐based polyurethane elastomer (Cu–DOU–CPU) with synergetic triple dynamic bonds is developed. Cu–DOU–CPU demonstrates the highest reported mechanical performance for self‐healing elastomers at room temperature, with a tensile strength and toughness up to 14.8 MPa and 87.0 MJ m−3, respectively. Meanwhile, the Cu–DOU–CPU spontaneously self‐heals at room temperature with an instant recovered tensile strength of 1.84 MPa and a continuously increased strength up to 13.8 MPa, surpassing the original strength of all other counterparts. Density functional theory calculations reveal that the coordination of Cu(II) plays a critical role in accelerating the reversible dissociation of dimethylglyoxime–urethane, which is important to the excellent performance of the self‐healing elastomer. Application of this technology is demonstrated by a self‐healable and stretchable circuit constructed from Cu–DOU–CPU.

Stretchable conductive fibers are key elements for next‐generation flexible electronics. Most existing conductive fibers are electron‐based, opaque, relatively rigid, and show a significant increase in resistance during stretching. Accordingly, soft, stretchable, and transparent ion‐conductive hydrogel fibers have attracted significant attention. However, hydrogel fibers are difficult to manufacture and easy to dry and freeze, which significantly hinders their wide range of applications. Herein, organohydrogel fibers are designed to address these challenges. First, a newly designed hybrid crosslinking strategy continuously wet‐spins hydrogel fibers, which are transformed into organohydrogel fibers by simple solvent replacement. The organohydrogel fibers show excellent antifreezing (< ‐80 °C) capability, stability (>5 months), transparency, and stretchability. The predominantly covalently crosslinked network ensures the fibers have a high dynamic mechanical stability with negligible hysteresis and creep, from which previous conductive fibers usually suffer. Accordingly, strain sensors made from the organohydrogel fibers accurately capture high‐frequency (4 Hz) and high‐speed (24 cm s−1) motion and exhibit little drift for 1000 stretch–release cycles, and are powerful for detecting rapid cyclic motions such as engine valves and are difficult to reach by previously reported conductive fibers. The organohydrogel fibers also demonstrate potential as wearable anisotropic sensors, data gloves, soft electrodes, and optical fibers.

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The bio-integrated electronics industry is booming and becoming more integrated with biological tissues. To successfully integrate with the soft tissues of the body (eg. skin), the material must possess many of the same properties including compliance, toughness, elasticity, and tear resistance. In this work, we prepare mechanically and biologically skin-like materials (PSeD-U elastomers) by designing a unique physical and covalent hybrid crosslinking structure. The introduction of an optimal amount of hydrogen bonds significantly strengthens the resultant elastomers with 11 times the toughness and 3 times the strength of covalent crosslinked PSeD elastomers, while maintaining a low modulus. Besides, the PSeD-U elastomers show nonlinear mechanical behavior similar to skins. Furthermore, PSeD-U elastomers demonstrate the cytocompatibility and biodegradability to achieve better integration with tissues. Finally, piezocapacitive pressure sensors are fabricated with high pressure sensitivity and rapid response to demonstrate the potential use of PSeD-U elastomers in bio-integrated electronics.

Preparing a biobased (biomass-based) high performance epoxy resin with extremely large biomass content is of great importance for sustainable development. Herein, a new epoxy resin with a precise structure, bis(2-methoxy-4-(oxiran-2ylmethyl)phenyl)furan-2,5-dicarboxylate (EUFU-EP), was synthesized from two biobased green and low toxic compounds (2,5furandicarboxylic acid and eugenol) and the biomass content of EUFU-EP is as large as 93.3%. In addition, a new biobased epoxy resin, EUFU-EP/MHHPA, was prepared by using methyl hexahydrophthalic anhydride (MHHPA) as the curing agent and 2ethyl-4-methylimidazole as the curing accelerator. The curing reactivity and integrated performances including thermal and mechanical properties as well as flame retardancy of the cured resin were systematically researched and compared with those of petrochemical resource-based epoxy resin (DGEBA/MHHPA) consisting of commercial diglycidyl ether of bisphenol A (DGEBA), MHHPA and 2-ethyl-4-methylimidazole. Results show that EUFU-EP/MHHPA and DGEBA/MHHPA have similar curing reactivity, but cured EUFU-EP/MHHPA resin shows better thermal properties, rigidity, and flame retardancy than cured DGEBA/MHHPA resin. Specifically, the glass transition temperature (T g ) of EUFU-EP/MHHPA resin is as high as 153.4 °C, the storage modulus at 50 °C increases by 19.8%; meanwhile, both peak heat release rate and total heat release reduce by 19.0%. The nature behind these outstanding integrated performances is attributed to the unique structure of EUFU-EP, which is not only rich in aromatic structure but also has a furan ring. The especially large biomass content and outstanding thermal, mechanical, and flame retarding performances clearly show that EUFU-EP resin has a great potential in actual applications.