Polymer‐based solid electrolytes (PSEs) offer great promise in developing lithium metal batteries due to their attractive features such as safety, light weight, low cost, and high processability. However, a PSE‐based lithium battery usually requires a relatively high temperature (60 °C or above) to complete charge and discharge due to the poor ionic conductivity of PSEs. Herein, a gel polymer electrolytes (GPEs) film with a supramolecular network structure through a facile one‐step photopolymerization is designed and developed. The crosslinked structure and quadruple hydrogen bonding fulfil the GPEs with high thermal stability and good mechanical property with a maximum tensile strain of 48%. The obtained GPEs possess a high ionic conductivity of 3.8 × 10−3 S cm−1 at 25 °C and a decomposition voltage ≥ 4.6 V (vs Li/Li+). The cells assembled with LiFePO4 cathode and Li anode, present an initial discharge specific capacity of 155.6 mAh g−1 and a good cycling efficiency with a capacity retention rate of 81.1% after 100 charges/discharge cycles at 0.1 C at ambient temperature. This work encompasses a route to develop high performance PSEs that can be operated at room temperature for future lithium metal batteries.

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Hydrogel-based wearable sensors have flourished as encouraging candidates for human mechanosensation due to their controllable conductivity and tailorable mechanical performances. However, it is still a great challenge to fabricate hydrogelbased wearable sensors with long-term durability and long service lifespan, while maintaining good sensing sensitivity and mechanical performances. This work demonstrates the formulation of a novel urushiol-induced hydrogel of exclusive microstructure and long-term durability by facile one-step copolymerization, and the development of hydrogel-based mechanosensors with brilliant durability, long lifespan, and long-term and robust adhesiveness in air and water. The hydrogel-based sensors possess extraordinary self-recovery capability and eminent synchronism between applied strains and output signals, which can contribute to the synergistic effect of the fast mobility of flexible polymer chains assigned by the flexible alkyl chains and the construction of an optimized energy dissipation mechanism endowed with molecular-scale dynamic interactions. Moreover, the obtained hydrogel-based sensors can detect mechanical strains and distinguish human motions with high sensitivity, stable electrical signal responsiveness, and good biocompatibility, and have potential applications as wearable sensors for human motion monitoring.

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