Delamination‐Resistant and Light‐Induced Shape‐Memory Supercapacitors for Wearable Devices

Abstract Shape‐memory supercapacitors (SMCs) offer promising energy solutions for powering wearable sensors and electronic devices, enabling form adaptability on moving bodies and objects. However, traditional SMCs require high temperatures for shape‐editing, posing safety risks for devices, and often suffer from delamination during repeated shape transformations. In this study, a new class of wearable supercapacitors is reported that combine light‐induced shape ‐ memory with strong interfacial adhesion, achieved through a rehydration‐based assembly strategy using hydrogel electrolytes and electrodes. Key to this advancement are cinnamate‐functionalized materials, which undergo reversible 2+2 photocycloaddition under ultraviolet light at different wavelengths, enabling repeatable shape reconfiguration under mild, ambient conditions. The interfacial adhesive stress between the electrode and electrolyte reaches up to 40 kPa, substantially improving structural integrity. The supercapacitors exhibit outstanding electrochemical performance, with capacitance retention rates of 98.6% and 94.8% after 5000 and 10 000 charge–discharge cycles, respectively – surpassing values reported in previous studies. Additionally, they maintain 96.8% capacitance after ten shape‐memory cycles and can be reconfigured into multiple shapes without performance loss. Demonstrations powering a light‐emitting diode and an electronic watch further highlight their practical applicability in wearable and flexible electronics.