Integrated nanoelectromechanical systems (NEMS) exhibit enormous potential for replacing current microelectromechanical systems in various fields, such as 5G/6G wireless communication, in the future. However, their advancement is impeded by the challenge of achieving nanometer-thick ferroelectric oxide films with a high piezoelectric coefficient of d33. Herein, the nm-thick flexible Hf0.5Zr0.5O2 (HZO) films were deposited on mica substrates, and they exhibited a remnant polarization of ≥ 8.1 μC/cm2 at 25–320 °C and a high d33 value of 37.8 pC/N at 25 °C. After the HZO films with inter-digitated electrodes were fully polarized, the flexible HZO film with a dynamic bending strain of 0.102 % at 4 Hz produced an open-circuit voltage of 1.1 V. This HZO film with strong piezoelectricity can promote the development of novel NEMS and flexible piezoelectric sensors.