A Highly Stretchable and Real‐Time Healable Supercapacitor

In addition to a high specific capacitance, a large stretchability and self‐healing properties are also essential to improve the practicality and reliability of supercapacitors in portable and wearable electronics. However, the integration of multiple functions into one device remains challenging. Here, the construction of a highly stretchable and real‐time omni‐healable supercapacitor is demonstrated by sandwiching the polypyrrole‐incorporated gold nanoparticle/carbon nanotube (CNT)/poly(acrylamide) (GCP@PPy) hydrogel electrodes with a CNT‐free GCP (GP) hydrogel as the electrolyte and chemically soldering an Ag nanowire film to the hydrogel electrode as the current collector. The newly developed dynamic metal‐thiolate (M‐SR, M = Au, Ag) bond‐induced integrated configuration, with an intrinsically powerful electrode and electrolyte, enables the assembled supercapacitor to deliver an areal capacitance of 885 mF cm−2 and an energy density of 123 µWh cm−2, which are among the highest‐reported values for stretchable supercapacitors. Notably, the device exhibits a superhigh stretching strain of 800%, rapid optical healing capability, and significant real‐time healability during the charge–discharge process. The exceptional performance combined with the facile assembly method confirms this multifunctional device as the best performer among all the flexible supercapacitors reported to date. A highly stretchable and real‐time omni‐healable supercapacitor is constructed by synergistically designing the entire device from the microstructures of the hydrogel electrode and electrolyte, to the interfacial interactions among the current collector, electrode, and electrolyte, and further to all‐in‐one device configuration via dynamic metal‐thiolate coordination chemistry. This supercapacitor shows great potential in the field of next‐generation flexible/wearable electronics.