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With the world’s focus on wearable electronics, the scientific community has anticipated the plasticine-like processability of electrolytes and electrodes. A bioinspired composite of polymer and phase-changing salt with the similar bonding structure to that of natural bones is a suitable electrolyte candidate. Here, we report a water-mediated composite electrolyte by simple thermal mixing of crystallohydrate and polymer. The processable phase-change composites have significantly high mechanical strength and high ionic mobility. The wide operating voltage range and high faradic capacity of the composite both contribute to the maximum energy density. The convenient assembly and high thermal-shock resistance of our device are due to the mechanical interlocking and endothermic phase-change effect. As of now, no other non-liquid electrolytes, including those made from ceramics, polymers, or hydrogels, possess all of these features. Our work provides a universal strategy to fabricate various thermally manageable devices via phase-change electrolytes.

Water-mediated crystallohydrate–polymer composite as a phase-change electrolyte