In this research, ZnO/ZnS core/shell nanostructures were grown by electro-hydrothermal methods on titanium substrates. To optimize the growth of the nanostructures, the ZnO seed layer electro-deposition time was adjusted to modify the surface of the nanostructure. Multiple material characterizations were performed to examine the surface morphologies and material properties of the nanostructures. Results indicate that ZnO/ZnS nanostructures with ZnO deposition time of 5 sec had well-grown ZnO nanorods and high-quality ZnS nanoparticles for ZnO/ZnS core shell structures. ZnO/ZnS nanostructures on titanium substrates show promising for future development of titanium substrate-based biomedical and optoelectronic devices in the future.