Flexible piezoelectric nanogenerators (F-PENG) as a clean, green power generation device have attracted much attention. Dielectrophoresis (DEP) was used to prepare flexible piezoelectric nanogenerators with necklace-like oriented structure. The results showed that the oriented structure significantly improved the electrical output performance of F-PENG by enhancing the stress and free charge transmission. For the F-PENG with 8 vol% oriented PZT particle, open-circuit voltage and short-circuit current reached 176 V and 35 mu A and an instantaneous power of up to 2 mW was collected for an optimal matched load resistance of 6 M omega. Output voltage and current increase by 135% and 133%, respectively, compared with the F-PENG with random structure. Meanwhile, the finite element simulation results also confirmed the superiority of this oriented structure. There was a clear linear relationship between the output voltage and pressure, and the sensitivity was 1.13 N/V. The oriented PZT particle-based F-PENG with excellent electrical output performance has great application prospects in the fields of green power generation and self-powered building monitoring system.