The ultra-thin II-VI semiconductor ZnS/ZnO bilayers (< 50 nm thickness for each layer) can be easily formed on the plastic substrates at 70˜80°C for 20 min. By low temperature wet chemical synthesis techniques, namely chemical bath deposition (CBD) and successive ionic layer adsorption and reaction (SILAR). The specific microstructure of such ZnS/ZnO bilayers including film thickness, particle size and morphology, is also modified and obtained in accordance with processing parameters. Along with thin film quality and morphology, the transmittance and reflectance of ZnS/ZnO layers can be measured by field emission SEM and UV-Vis spectroscopy. Besides the bilayer of ZnS (˜35 nm thick)/ZnO (˜50 nm thick) film with uniform thickness was successfully deposited on the optical grade PET substrates, a well-distributed layer of ZnO nanoparticles with ˜100 nm size on the top of ZnS (35 nm thick) film was also attempted. The average transmittance of these bilayer samples can reach greater 85%. Our future goal is to employ such ZnS/ZnO bilayer structure on potential organic substrates to be associated with flexible photovoltaic devices to meet desired cost-effectiveness requirements.