Flexible piezoelectric nanogenerator (PENG) and triboelectric nanogenerators (TENG) have gained prodigious attention due to the increasing demand of nano and micro energy for driving of miniaturized electronic devices, sensors, and various internet of things. The key challenges that are currently in focus are material selection and simple fabrication techniques for improved electrical performance along with good mechanical properties and flexibility. Herein, a ferroelectric polymer, poly(vinylidenefluoride-co-trifluoroethyne) (PVDF-TrFE), is chosen as a flexible material due to its promising prospect for energy harvesting. To improve the performance, a ceramic material, 0.65Pb(Mg1/3Nb2/3)O3–0.35PbTiO3 (PMN-PT), with very high piezoelectric properties has been selected as the reinforcement. Further, reduced graphene oxide has been added as a conducting filler to promote charge conduction. A remarkable enhancement in output voltage of nearly 3 fold is achieved in PVDF-TrFE/PMN-PT (PP) polymer composite as compared to the base polymer PVDF-TrFE (P) TENG device. Furthermore, the PVDF-TrFE/rGO/PMN-PT (PPR) as a PENG illustrates a great improvement in output current of the order of 2 as compared to the pristine polymer. The maximum output voltage as shown by the TENG is 200 V and the maximum current that is shown by the PENG is 30 µA. Therefore, the fabricated PMN-PT based PVDF-TrFE nanogenerators have an immense prospect for applications in self-powered systems.