We report high performance flexible piezoelectric nanogenerators (PENGs) by employing vanadium (V)-doped ZnO nanosheets (NSs) and the polydimethylsiloxane (PDMS) composite structure. The V-doped ZnO NSs were synthesized to overcome the inherently low piezoelectric properties of intrinsic ZnO. Ferroelectric phase transition induced in the V-doped ZnO NSs contributed to significantly improve the performance of the PENGs after the poling process. Consequently, the PENGs exhibited high output voltage and current up to ∼32 V and ∼6.2 μA, respectively, under the applied strain, which are sufficient to directly turn on a number of light emitting diodes (LEDs). The composite approach for PENG fabrication is scalable, robust, and reproducible during periodic bending/releasing over extended cycles. The approach introduced here extends the performance limits of ZnO-based PENGs and demonstrates their potential as energy harvesting devices.