Films of piezoelectric poly(vinylidene fluoride) (PVDF) and its copolymer P(VDF-TrFE) have been studied intensively for their potential application in piezoelectric sensing devices. The present work focuses on tuning the piezoelectric properties of P(VDF-TrFE) films via incorporating Ag and polydopamine co-decorated PZT (Ag@PDA@PZT) particles. Ag@PDA@PZT particles can effectively improve the β-phase content and piezoelectric properties of P(VDF-TrFE) films. The highest open-circuit voltage and short-circuit current of P(VDF-TrFE)-based flexible pressure sensors incorporating Ag@PDA@PZT particles are ~30 V and ~2.4 μA, respectively. The flexible sensors exhibit a response to different body movements, providing a practical and potentially useful basis for human−machine interface applications.