The results of these mechanical and electrical tests provide detailed insights into how PLLA films respond to specific types of mechanical stimuli. The strain test, depicted in Figure , evaluated the films' piezoelectric response to cyclic stretching. Each mechanically deformed film was subjected to a 5% uniaxial strain under controlled conditions, enabling a systematic assessment of their ability to generate electrical output under mechanical deformation. The results of this test, including the output voltage and current, are presented in Figure . Unprocessed films exhibited negligible piezoelectric activity, confirming that mechanical deformation is essential to activate the material's piezoelectric potential. This is attributed to the isotropic molecular orientation and lower crystallinity of unprocessed films, where the dipole moments are randomly distributed, resulting in a near-zero net dipole moment. Mechanical stretching induces molecular alignment and transitions from the α-phase to the β-phase, where dipoles align along the polymer chain backbone, significantly enhancing the material's piezoelectric properties . In contrast, 50%, 75%, and 100% strained films displayed progressively higher piezoelectric outputs. The 50% strained film generated a peak-to-peak voltage of approximately 7.1V (±0.2V) and a current of 0.31 nA (±0.06 nA), while the 75% strained film produced around 19.3V (±0.5V) and 138.8 nA (±25.1 nA). The 100% strained films demonstrated the highest performance, with a peak-to-peak voltage of 23.8V (±0.4V) and a current of 203.8 nA (±24.9 nA). These results align with structural analyses indicating that uniaxial stretching induces the formation of the β-phase crystalline structure, enhancing molecular alignment and dipole density, which are critical for improved piezoelectric activity. The experimentally confirmed molecular orientation, as determined through THz spectroscopy in our previous work , underscores the importance of cutting the films at a 45-degree angle relative to the strain direction. This specific orientation ensures the optimal alignment of molecular dipoles with mechanical input, maximizing the activation of piezoelectric pathways and highlighting the critical role of precise molecular arrangement in achieving superior performance.