Zirconium diselenide thin films were electrodeposited on the stainless steel substrates for various pH values ranging from 2.0 to 3.5. The deposition potential range suitable for the deposition has been optimized using cyclic voltammetry (CV). The X-Ray Diffraction (XRD) results confirm that the thin films produced were polycrystalline in nature with hexagonal structure peak at 2θ = 43.8° (003) of ZrSe2. The surface morphology of the film indicate, as the pH was increased the grain size of the film become larger due to agglomeration. The direct band gap energy of the films was found to be in the range of 1.77–1.83 eV.