Developing flexible energy storage devices with the ability to retain capacitance under extreme deformation is promising but remains challenging. Here, we report the development of a durable supercapacitor with remarkable capacitance retention under mechanical deformation by utilizing a physical double-network (DN) hydrogel as an electrolyte. The first network is hydrophobically associating polyacrylamide cross-linked by nanoparticles, and the second network is Zn2+ cross-linked alginate. Through soaking such a DN hydrogel into a high concentration of ZnSO4 solution, a highly deformable electrolyte with good conductivity is fabricated, which also shows adhesion to diverse surfaces. Directly attaching the hydrogel electrolyte to two pieces of an active carbon cloth facilely produces a flexible supercapacitor with a high specific capacitance and theoretical energy density. Remarkable capacitance retention under tension, compression, and bending is observed for the supercapacitor, which can also maintain above 87% of the initial capacitance after 4000 charge–discharge cycles. This study provides a simple way to fabricate hydrogel electrolytes for deformable yet durable supercapacitors, which is expected to inspire the development of next-generation flexible energy storage devices.

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