To apply thin ZnO film to photoacoustic tomography sensors, we investigated methods to improve its piezoelectricity with high optical transmittance. ZnO film was deposited by RF magnetron sputtering on a quartz substrate with various changes of the following conditions: RF sputtering power, Ar gas pressure, and substrate temperature (TSUB). The preliminary optimization of sputtering conditions is to form the ZnO film with good c-axis crystalline alignment. The results of X-ray diffraction measurement and cross-sectional observations indicated that the high-TSUB condition was preferable. This was because the desorption of Zn due to high-TSUB during the deposition process induced the formation of excellent columnar grains normal to the substrate. To enhance the piezoresponse, the substitution of Zn with different crystal-radius atoms was investigated, the aim being to increase the electrically neutral dipole moment by the partial displacement of the Zn-O bond. The transition metal V, with the potential to have the various configurations and coordination numbers, was selected as the dopant. As a result, it was confirmed that the diffraction peak from the (002) plane shifted to low angles with small degradation of the diffraction intensities.