Nowadays, wearable and flexible nanogenerators are of great importance for portable personal electronics. A flexible piezoelectric energy harvester (f-PEH) based on Bi_3.15Nd_0.85Ti₃O₁₂ single crystalline nanoplates (BNdT NPs) and polydimethylsiloxane (PDMS) elastomeric polymer was fabricated, and high piezoelectric energy harvesting performance was achieved. The piezoelectric output performance is highly dependent on the mass ratio of the BNdT NPs in the PDMS matrix. The as-prepared f-PEH with 12.5 wt% BNdT NPs presents the highest output voltage of 10 V, a peak-peak short-circuit current of 1 μA, and a power of 1.92 μW under tapping mode of 6.5 N at 2.7 Hz, which can light up four commercial light emitting diodes without the energy storage process. The f-PEHs can be used to harvest daily life energy and generate a voltage of 2–6 V in harvesting the mechanical energy of mouse clicking or foot stepping. These results demonstrate the potential application of the lead-free BNdT NPs based f-PEHs in powering wearable electronics