In this study, bimetallic cobalt-vanadium-based layered double hydroxide (CoV-LDH) systems were developed by varying the Co/V molar ratios (1:1 and 2:1) and hydrothermal temperatures (120 and 180 °C). Structural analysis by X-ray diffraction (XRD), Raman, and Fourier-transform infrared (FTIR) spectroscopy indicated the successful formation of CoV-LDH with a unique structure and lattice distortions, reflecting the influence of both the metal concentrations and temperature on the crystal and chemical structures of the developed bimetallic systems. Similarly, the field-emission scanning electron microscopy (FESEM) and high resolution transmission electron microscopy (HRTEM) images revealed a flaky 2D nanosheet-like structure for the bimetallic CoV-LDH with a 1:1 ratio prepared at 120 °C (CVL1-120), whereas one-dimensional (1D) and three-dimensional (3D) morphologies were observed for other bimetallic CoV-LDH systems prepared with a different molar ratio (2:1) and/or temperature (180 °C). Electrochemical analysis performed in a three-electrode setup demonstrated a specific capacitance of 314.4 F g