With the energy shortage and the increasing awareness of environmental protection, piezoelectric nanogenerator (PENG) has been widely studied in recent years. Polyvinylidene fluoride hexafluoropropylene (P(VDF-HFP)) is an ideal matrix material because of its piezoelectricity, flexibility, and toughness.Herein, a composite film of carbon nanotubes (CNTs), Ba 0.85 Ca 0.15 Zr 0.10-Ti 0.90 O 3 (BCZT), and P(VDF-HFP) (CNTs/BCZT/P(VDF-HFP)) were prepared via the tape casting method. Adding BCZT increased the polar β-phase in P(VDF-HFP), reaching a maximum when 40 wt% BCZT was incorporated.Adding CNTs to the matrix provides a conductive path inside the composite. The CNTs/BCZT/P(VDF-HFP) composite film demonstrated optimal electrical properties when 0.3 wt% CNTs is doped, with the open circuit voltage increased from 22 to 30 V and the short circuit current increased from 3 to 5.9 μA compared with the undoped sample. The output performance of the PENG was further improved with a three-layer folded structure, achieving an open circuit voltage of 40 V and a maximum power density of 31.5 mW m À2 , which easily lit six light-emitting diodes.