One‐Step Scalable Fabrication of Graphene‐Integrated Micro‐Supercapacitors with Remarkable Flexibility and Exceptional Performance Uniformity

Abstract The rapid development of miniature electronics has accelerated the demand for simplified and scalable production of micro‐supercapacitors (MSCs); however, the preparation of active materials, patterning microelectrodes, and subsequent modular integration of the reported MSCs are normally separated and are involved in multiple complex steps. Herein, a one‐step, cost‐effective strategy for fast and scalable fabrication of patterned laser‐induced graphene (LIG) for all‐solid‐state planar integrated MSCs (LIG‐MSCs) with various form factors of designable shape, exceptional flexibility, performance uniformity, superior modularization, and high‐temperature stability is demonstrated. Notably, using the conductive and porous LIG patterns composed of randomly stacked graphene nanosheets simultaneously acting as both microelectrodes and interconnects, the resulting LIG‐MSCs represent typical electrical double capacitive behavior, having an impressive areal capacitance of 0.62 mF cm −2 and long‐term stability without capacitance degeneration after 10 000 cycles. Furthermore, LIG‐MSCs display exceptional mechanical flexibility and adjustable voltage and capacitance output through arbitrary arrangement of cells connected in series and in parallel, indicative of exceptional performance customization. Moreover, all‐solid‐state LIG‐MSCs working at ionogel electrolyte exhibit highly stable performance even at high temperature of 100 °C, with 90% capacitance retention over 3000 cycles, suggestive of outstanding reliability. Therefore, the LIG‐MSCs offer tremendous opportunities for miniature power source‐integrated microelectronics.