ZnO/ZnS heterostructures were synthesized by a two steps electrochemical deposition method. Firstly, ZnS layer was deposited from an aqueous solution containing Na2S2O3 and ZnSO4 onto indium-doped tin oxide (ITO) coating glass substrate at two deposition potentials. Then, ZnO nanostructures were deposited from an aqueous solution of Zn(NO3) onto ZnS surface. The as-obtained samples were characterized by scanning electron microscopy (SEM), atomic force microscopy (AFM), X-ray diffraction (XRD), Raman and UV-visible analysis. The results indicate that the electrodeposition of ZnS layer at −0.9 V give the best proprieties of ZnO/ZnS heterostructures. Homogeneous and uniform surface of ZnO/ZnS heterostructure was confirmed by AFM images. The XRD patterns indicates a high crystallinity of ZnO/ZnS. A high transmittance of 65% was also noted from UV-Visible spectra and band gap energy as large as 3.6 eV was found.