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Multiple stretchability has never been demonstrated as supercapacitors because the hydrogel used cannot fully recover after being heavily deformed. Now, a highly reversibly stretchable all‐polymer supercapacitor was fabricated using a developed double network hydrogel (DN hydrogel) as electrolyte and pure polypyrrole (PPy) as electrode. The DN hydrogel provides excellent mechanical properties, which can be stretched up to 500 % many times and then restore almost 100 % of the original length. To fabricate the fully recoverable stretchable supercapacitor, we annealed a free‐standing pure conducting polymer film as electrode so that the electrodes induced retardance is minimized. The as‐fabricated DN hydrogel/pure conducting polymer supercapacitors can be perfectly recovered from 100 % strain with almost no residual deformation left and the electrochemical performance can be maintained even after 1000 stretches (but not bending). [ABSTRACT FROM AUTHOR]

Stretchability and compressibility of supercapacitors is an essential element of modern electronics, such as flexible, wearable devices. Widely used polyvinyl alcohol-based electrolytes are neither very stretchable nor compressible, which fundamentally limits the realization of supercapacitors with high stretchability and compressibility. A new electrolyte that is intrinsically super-stretchable and compressible is presented. Vinyl hybrid silica nanoparticle cross-linkers were introduced into polyacrylamide hydrogel backbones to promote dynamic cross-linking of the polymer networks. These cross-linkers serve as stress buffers to dissipate energy when strain is applied, providing a solution to the intrinsically low stretchability and compressibility shortcomings of conventional supercapacitors. The newly developed supercapacitor and electrolyte can be stretched up to an unprecedented 1000 % strain with enhanced performance, and compressed to 50 % strain with good retention of the initial performance. [ABSTRACT FROM AUTHOR]