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Manganese oxides/graphene is an electrode material currently under consideration for use in high-performance supercapacitors (SCs). The conventional, widely used wet chemical methods for preparing MnO2/graphene are tedious and consume large quantities of strong reduction/oxidation reagents. The resulting powder composites require adhesives to form a suitable electrode. In the present study, we report on a method for synthesizing MnO2/graphene composite electrodes using a second laser irradiation employing a laser of the polyether ether ketone. This simple and environmentally friendly method allows the patterning of electrodes together with the synthesis of the active materials. The MnO2/laser-induced graphene (LIG) electrode exhibited a high capacitance of 48.9 mF cm−2, which is about 2.4 times greater than a pure LIG electrode. Assembled all solid micro-supercapacitors (MSCs) containing the novel LIG electrodes delivered both high energy density (3.1 μWh cm−2) and power density (2.5 mW cm−2). These MSCs exhibited a capacitance retention of 94.3% over 3000 cycles, at a current density of 0.5 mA cm−2. The electrochemical performance was almost unaltered by bending the MSC to 150°. This method of synthesizing high-performance flexible electrodes is important for future development of wearable electronics. [ABSTRACT FROM AUTHOR]