Piezoelectric Poly (vinylidene fluoride) (PVDF) films with high flexibility are a suitable and promising replacement for rigid ceramic piezoelectric materials. However, for this purpose, enhancing piezoelectric properties and adopting an industrial fabrication method are of great importance. In this study, 5–9 µm thick PVDF films were fabricated by a nozzle-less ultrasonic spray coating (USC) system, followed by an annealing process at 100 °C. By applying proper spraying parameters, we could obtain highly uniform films with large d33 values (48 pm/V) and 56% crystallinity. Results show that the uniformity of the films plays an important role in the final piezoelectric properties. Thus, ultrasonic spray coating method can be used for fabrication of large-scale piezoelectric films with no need for poling or stretching processes.