This work used a highly flexible, sustainable polyimide tape as a substrate to deposit ductile-natured carbonaceous Ni 3 N (C/Ni 3 N@polyimide) material for supercapacitor application. C/Ni 3 N was prepared using a co-sputtering technique, and this method also provided better adhesion of the electrode material over the substrate, which is helpful in improving bending performance. The ductile behavior of the sputter-grown electrode and the high flexibility of the polyimide tape provide ultimate flexibility to the C/Ni 3 N@polyimide-based supercapacitor. To achieve optimum electrochemical performance, a series of electrochemical tests were done in the presence of various electrolytes. Further, a flexible asymmetric supercapacitor (NC-FSC) (C/ Ni 3 N//carbon@polyimide) was assembled by using C/Ni 3 N as a cathode and a carbon thin film as an anode, separated by a GF/C-glass microfiber soaked in optimized 1 M Li 2 SO 4 aqueous electrolyte. The NC-FSC offers a capacitance of 324 mF cm −2 with a high areal energy density of 115.26 μWh cm −2 and a power density of 811 μW cm −2 , with ideal bending performance.