For ZnO/diamond structured surface acoustic wave (SAW) filters, performance is sensitively dependent on the quality of the ZnO films. In this paper, we prepare highly-oriented and fine grained polycrystalline ZnO thin films with excellent surface smoothness on the smooth nucleation surfaces of freestanding CVD diamond films by metal organic chemical vapour deposition (MOCVD). The properties of the ZnO films are characterized by x-ray diffraction (XRD), scanning electron microscopy (SEM), and photoluminescence (PL) spectrum. The influences of the deposition conditions on the quality of ZnO films are discussed briefly. ZnO/freestanding thick-diamond-film layered SAW devices with high response frequencies are expected to be developed.