In this work, poly (vinylidene fluoride)/protein composite films are prepared which is free standing and flexible. Nucleation of electroactive β-phase in poly (vinylidene fluoride) (PVDF) and consecutive surface morphological changes with different weight percentage of protein is systematically investigated. Finally, the PVDF/protein composite film is used to make a mechanical energy harvesting device. The flexible device produces 2.5 V open-circuit voltage under repeated hand punching. Thus, the device can be used for self-powered consumer electronics in near future.