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Novel all-solid-state microsupercapacitors (MSCs) with three-dimensional (3D) electrodes consisting of active materials (ie, graphene or activated carbon (AC) particles) and polymer electrolyte (PE) designed for high-energy-density storage applications were fabricated and tested in this work. The incorporation of PE in the electrode material enhances the accessibility of electrolyte ions to the surface of active materials and decreases the ion diffusion path during electrochemical charge/discharge. For a scan rate of 5 mV s− 1, the MSCs with graphene/PE and AC/PE composite electrodes demonstrate a very high areal capacitance of 95 and 134 mF cm− 2, respectively, comparable to that of 3D MSCs with liquid electrolyte. In addition, the graphene/PE MSCs show a∼ 70% increase in specific capacitance after 10 000 charge/discharge cycles, attributed to an electro-activation process resulting from ion intercalation …