In this study, we developed a method to combine polyamic acid (PAA) and activated carbon (AC), which were then coated on laser-induced graphene (LIG). The material was heated to facilitate the conversion of PAA–AC into polyimide (PI)–AC. Then, the resulting material was subjected to a second laser irradiation process to obtain AC–LIG composite materials. The resulting material features a robust and flexible electrode architecture with a high surface area, improved ion accessibility, and enhanced charge transfer kinetics. In tests conducted with a three-electrode setup, the AC–LIG configuration exhibited a considerably high specific capacitance, reaching 97.2 mF cm−2 at 0.2 mA cm−2, which is approximately fourteen times larger than that of pristine LIG (7.1 mF cm−2). When integrated into a flexible microsupercapacitor using a polyvinyl alcohol (PVA)–H2SO4 (sulfuric acid) gel-type electrolyte, AC–LIG exhibited a higher specific capacitance (68.4 mF cm−2 at 0.3 mA cm−2) than d-LIG (17.1 mF cm−2 at 0.3 mA cm−2). Furthermore, AC–LIG showed good Coulombic efficiency (98.5 %) and capacitance retention (90.0 %) after 10,000 cycles. These results highlight the potential of AC–LIG as a viable alternative for advanced supercapacitor (SC) applications, providing improved energy storage capacities and a reliable performance.