ZnO was electrodeposited on single-crystal, highly (111) textured polycrystalline, and randomly aligned polycrystalline Au films serving as the cathodes. The electrodeposition was carried out in a zinc nitrate aqueous solution at . The morphologies and crystal structures of ZnO were closely related to the properties of the Au surface. A detailed analysis was conducted, and the conclusion is that while the structural properties of ZnO can be controlled by controlling the crystal properties of Au film, the optical properties of ZnO are similar under the same electrodeposition conditions. However, using a two-step electrodeposition, smooth and compact epitaxial ZnO films are obtained.