Recent advances in energy harvesting have enabled efficient conversion of mechanical and light energy into electricity, with piezoelectric and photo-assisted hybrid strategies emerging as key drivers for flexible, high performance, and eco-friendly self-powered systems. In this study, we demonstrate a straightforward strategy to stabilize α-formamidinium lead iodide (α-FAPbI₃) by embedding it within a polyvinylidene fluoride (PVDF) matrix, yielding a stable composite film as confirmed by X-ray diffraction (XRD) analysis. Composite films of α-FAPbI₃ and PVDF were prepared in varying ratios and systematically optimized by evaluating their ferroelectric behavior, including saturation polarization, remnant polarization, and energy storage density. Among these, 210 μL of α FAPbI₃ in 1 g PVDF (FPF-3 composition) exhibited the most optimized performance. The photoactivity of the stabilized α-phase FAPbI₃, coupled with the intrinsic piezoelectric properties of PVDF, offers a synergistic platform for advanced photo-assisted energy harvesting applications. The photo-assisted energy harvesting device fabricated from the optimized composite exhibited distinct output variations under dark conditions, white light, and ultraviolet (UV) light exposure (360 nm and 390 nm), highlighting its potential for photo-assisted energy harvesting. Notably, a ~62.02% enhancement in output voltage was achieved under white light illumination. The optimized light-assisted device exhibited remarkable output enhancement, highlighting its potential as a promising candidate for next-generation self-powered energy systems.

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