• Laser-produced graphene (LPG) from polyimide via CO2 laser irradiation yields multilayer graphene with sp2 C=C bonds and 3D sheet-like morphology.
• LPG electrodes exhibit high areal capacitance of 51 mF cm−2 (170 F g−1) at 1 mA cm−2 in 1 M KOH, with energy density ~3.5 µWh cm−2 and power density ~350 µW cm−2.
• Excellent cycling stability: 87% capacitance retention after 3,000 cycles in three-electrode configuration, and superior retention after 10,000 cycles in symmetric device.
• Symmetric supercapacitor using LPG electrodes achieves specific capacitance of 23 mF cm−2, demonstrating practical potential for energy storage applications.