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Hydrogel electrolytes have high room-temperature conductivity and can be widely used in energy storage device. However, hydrogels suffer from the inevitable freezing of water at subzero temperatures, resulting in the diminishment of their conductivity and mechanical properties. How to achieve high conductivity without sacrificing hydrogels' flexibility at subzero temperature is an important challenge. To address this challenge, a new type of zwitterionic polymer hydrogel (polySH) electrolytes is fabricated. The anionic and cationic counterions on the polymer chains facilitate the dissociation of LiCl. The antifreezing electrolyte can be stretched to a strain of 325% and compressed to 75% at −40 °C and possesses an outstanding conductivity of 12.6 mS cm −1 at −40 °C. A direct hopping migration mechanism of hydrated lithium-ion through the channel of zwitterion groups is proposed. The polySH electrolyte-based-supercapacitor (SC) exhibits a high specific capacitance of 178 mF cm −2 at 60 °C and 134 mF cm −2 at −30 °C with a retention of 81% and 71% of the initial capacitance after 10 000 cycles, respectively. The overall merits of the electrolyte will open up a new avenue for advanced ionic conductors and energy storage device in practical applications.

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