In this research, we propose a piezoelectric polymer multilayer coating method by solution casting and spin coating to improve the fabrication yield and piezoelectricity of the vibration energy harvester (VEH). The proposed multilayer coating method improves the smoothness of the surface of the piezoelectric layer and the device fabrication yield. To confirm the validity of the proposed coating method, we fabricated and compared four types of VEHs with different numbers of piezoelectric layers coated on a Cu/polyimide film. As a result of the evaluation, the piezoelectric characteristics and the fabrication yield of the coated film were found to be improved with increasing number of coating layers. In addition, because of the decrease in the film thickness per coating, the amount of output power generated by the fabricated piezoelectric VEH (PVEH) was increased.