In this research, a facile and cost-effective method of graphene synthesis by the modified carburization process and its applications for supercapacitor electrodes is reported. In this simple approach, carbon was diffused into nickel foam and naturally cooled to obtain carbon precipitation for the in situ growth of graphene by decarburization. Phase-structure and surface-morphology analysis revealed the presence of a highly reduced structure of the graphene layer. Furthermore, the large-intensity D, substantial G, and 2D bands in Raman spectra were attributed to disordered multilayer graphene. The three-electrode systems were used to measure electrochemical efficiency. The electrode sample exhibited enhanced current density of 0.6 A/g, electrode energy of 1.0008 Wh/kg, and power density of 180 W/kg, showing significant electrochemical performance for supercapacitor electrode applications.