Piezoelectric materials are highly valued for converting mechanical energy in electrical energy and vice versa, making them crucial for sensor and energy harvesting applications. This study focuses on fabricating low-cost piezoelectric films using polylactic acid (PLA) and PLA with zinc oxide (ZnO) nanoparticles (PLZnO). Different concentrations of ZnO (5, 10, 15, 20, and 40 wt%) were added the PLA structure. The films were created using solution casting technology, and their piezoelectric properties were analyzed. Electromechanical tests showed ZnO nanoparticles significantly improved the piezoelectric performance of films. Increased ZnO content led to better sensor sensitivity and electromechanical coupling. The highest performance under a 1 kgf impact pulse pressure at 3 Hz found in PLA–ZnO ilms with 20 wt% ZnO, with normalized peak-to-peak open circuit voltages and short-circuit current values of 8.55 Vpp/g and 167.1 nApp/g, respectively. Scanning electron microscopy (SEM) revealed a uniform ZnO nanoparticle distribution within the PLA matrix. Pure PLA exhibited peaks corresponding to the α-form crystal structure, indicating its semi-crystalline nature, while presence of amorphous regions was shown by peak broadening. Adding ZnO nanoparticles introduced additional peaks for ZnO’s crystalline structure. Overall, ZnO nanoparticles in PLA enhanced piezoelectric properties, making these films promising for sensor and energy harvesting applications. This study offers insights in developing eco-friendly and sustainable piezoelectric materials with the potential for future technological advancements.