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Aligned P(VDF-TrFE) nanofibers are successfully fabricated by advanced electrospinning. The aligned feature of the nanofibers is achieved by using parallel electrodes, which is fabricated by lithography and wet etching, and a rotating drum collector. Scanning electron microscope (SEM) images show that the nanofibers are highly ordered with a smooth surface and uniform diameter. X-ray diffraction (XRD) and Fourier Transform Infrared spectrum (FTIR) tests indicate that the fibers contain high β phase content. The nanogenerator based on aligned P(VDF-TrFE) nanofibers exhibits good electric performance with a maximum output voltage as high as 12 V and peak-peak short circuit current about 150 nA, highlighting the potential application of P(VDF-TrFE) on self-powered and wearable devices.