PVDF-TrFE-based wearable nanogenerators were designed and fabricated with enhanced performances via reduced graphene oxides (rGO) and in situ electric polarization. Our laboratory-made polarization system may complete the in situ poling of PVDF-TrFE films in 5 min without heating, which has the advantages of high production efficiency, excellent piezoelectric performances, and favorable uniformity, compared to traditional poling approaches. The addition of rGO into PVDF-TrFE significantly improved the crystallinity of the β-phase PVDF-TrFE and enhanced the formation of hydrogen bonds via interaction of dipoles between rGO and PVDF-TrFE. This further improved the energy-harvesting performances of these piezoelectric nanogenerators with 1.6 times of the open-circuit voltage and 2 times of the power density than that of pure PVDF-TrFE-based devices. The high production efficiency and excellent piezoelectric performances of in situ polarized rGO/PVDF-TrFE make them of great potential for self-powered, wearable/portable devices.