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In recent years, lead-free perovskite materials are exponentially emerging in photovoltaic and optoelectronic applications due to their low toxicity and superior optical properties. On the other hand, the demand for flexible, wearable, and lightweight optoelectronic devices is significantly growing in sensor and actuator technologies. In this scenario, lead-free perovskite-based flexible piezoelectric polymer composites have sparked considerable attention in this field due to their excellent piezo-, pyro-, ferroelectric, and photovoltaic properties. Thus, in this work, a long-term stable lead-free Cs 3 Bi 2 I 9 -PVDF composite is introduced. The in situ growth of the Cs 3 Bi 2 I 9 perovskite induces 92% yield of the electroactive phase in the PVDF matrix. The possible mechanism behind the electroactive β-phase transformation is presented via interfacial interactions of PVDF moieties with the Cs 3 Bi 2 I 9 (CBI) perovskite, which also give rise to long-term environmental stability. Next, a piezoelectric nanogenerator (PNG) has been fabricated with the Cs 3 Bi 2 I 9 -PVDF composite for mechanical energy harvesting, biophysiological motion monitoring, and voice recognitions that have potential utility in the health-care sector. Furthermore, a photodetector is developed to realize the piezophototronic effect. It exhibits a fast photoswitching behavior with rise and decay times of 141 and 278 ms, respectively. Thus, it is confirmed that the flexible Cs 3 Bi 2 I 9 -PVDF composite has shown tremendous potential to be used as an optical signal-modulated piezo-responsive wearable sensor.