There is a desperate demand for efficient energy storage systems to fulfill future energy demands. Herein, we exemplify a facile solvothermal approach followed by heat treatment to synthesize NiO/g-C3N4 nanocomposites for enhanced supercapacitor applications. The molar ratio of g-C3N4 is varied to achieve numerous nanostructures like nanoparticles and nanorods with optimum specific capacitance. Further, all as-prepared electrode materials are examined for supercapacitor application. The electrochemical behavior of prepared NiO/g-C3N4 nanocomposites is carried out under cyclic voltammetry (CV), galvanostatic charge-discharge (GCD), and electrochemical impedance spectroscopy (EIS) in a three-electrode cell under different electrolytes such as aqueous sodium sulphate electrolyte (1.0 M Na2SO4) and potassium hydroxide electrolyte (3.0 M KOH). Among all the electrode materials, NO-4 (1 : 2) shows the highest specific capacitance of 338.68 F/g at a scan rate of 2 mV/s and 161.3 F/g at a current density of 1 A/g in 1.0 M Na2SO4 electrolyte. Also, this electrode material shows 95.22 F/g at a scan rate of 2 mV/s in 3.0 M KOH electrolyte. The excessive specific capacitance of this electrode material is due to retarded charge transfer resistance in the interface at the electrode and electrolyte and a increased number of active sites. The investigation of the electrokinetics of all the prepared electrodes was also carried out, and it revealed the charge storage contribution of capacitive and diffusive parts which levitates the higher specific capacitance. The two-electrode study for evaluating supercapacitor performance is studied. The NO-4//NO-4 SSD in 1.0 M Na2SO4 electrolyte shows 18.23 F/g at a specific capacitance of 1 A/g with a corresponding energy density of 10.13 Wh/kg and a power density of 1.01 kW/kg, respectively.