Due to the severe environmental pollution and shortage of energy resources, the development of green energy has emerged drastically. In this study, the low-cost and lowpollution electrochemical deposition method was used to prepare non-toxic zinc oxide films on brass substrates, and piezoelectric devices were fabricated by zinc oxide with the piezoelectric properties to convert mechanical energy into electrical energy. In the results, the zinc oxide films prepared on the brass substrate were produced with the structures of nanorods. With the increases of the deposition voltage and deposition time, the alignment, morphological symmetry, and crystallinity of the zinc oxide nanorods could be effectively improved. By tuning the deposition voltage and electrolyte concentration, the surface morphology and the growth direction of zinc oxide could be well controlled. In addition, the annealing with the temperature of 400°C and 500°C could reduce the crystal defects and improve the crystallinity of zinc oxide. Finally, in the tests of piezoelectric devices, it could be observed that when the crystallinity of the zinc oxide (002) peak is improved, the output capability of the piezoelectric device could be increased simultaneously. While 2.350 V and 0.025 M Zn(NO3)2 + 0.025 MHMTA was used as the deposition voltage and the electrolyte in a electrochemical deposition on brass substrate for 2 hours, a device with the best piezoelectric property could be obtained. Furthermore, the subsequent annealing could significantly improve the crystallinity of the zinc oxide film. However, due to the influence of the mechanical properties of the substrate, the output capability of the piezoelectric device could not be achieved.