Piezoelectric composites have attracted significant research interest as sustainable power sources for electronic devices due to their high mechanical stability and electrical output characteristics. This study investigated the optimal processing conditions for fabricating a flexible piezoelectric energy harvester based on Pb(Zr,Ti)O3 (PZT) powder and a polyimide (PI) matrix composite. Various parameters, including the optimal mixing ratio of PI/PZT, ultrasonic treatment, homogenization, vacuum oven, and UV/O3 treatment, were optimized to achieve a uniform piezoelectric composite. A PZT content of 30 wt% and 20 minutes of homogenization were identified as the most effective conditions for increasing the uniformity of the composite. The optimized composite exhibited a high piezoelectric coefficient, a typical P-E hysteresis loop, and dielectric properties, exhibiting a voltage output that adjusts in response to variations in the applied touch force. This study provides foundational data for the uniform fabrication of flexible piezoelectric energy harvesters and next-generation miniaturized electronic devices.