Supercapacitors have garnered significant attention as one the most important energy storage devices due to their high-power density and greater cycling stability compared to the batteries. Following the graphene revolution in science, graphene analogs derived from other layered minerals with graphene-like structures, particularly ultrathin nanosheets of transition metal dichalcogenides with single or few atomic layers, have attracted an intense attention in the scientific community. In the present study, nanostructures of cobalt di-selenide chalcogenide were chemically engineered using tetra-ethylene pentaamine (TEPA), stabilized on a nickel foam substrate via the hydrothermal method at 160 °C, and utilized as an electrode material in supercapacitors. The TEPA entered the interlayer spacing of the synthesized chalcogenide and increased that spacing after removal of TEPA. Thus, the increased and engineered interlayer spacing will facilitate the ion insertion/de-insertion into chalcogenide structure, leads to enhanced stability and specific capacitance. Moreover, scanning electron microscopy (SEM) images showed holes and layers in the nanostructure which increases the active surface area of the electrode materials and thus enhancing the ions movement and efficiency. The modified electrode material was analyzed and exhibited a specific capacitance of 1310 F/g at a current density of 2 A/g. Our investigations of the current research project revealed that the modification and structural engineering of the nanomaterials can effectively produce the appropriate electrode materials towards the energy storage through high-performance supercapacitors.