The carbon nanotube / poly-vinylidene fluoride (CNT/PVDF) composite films for the nano-generator devices were fabricated by spray coating method using the CNT/PVDF solution, which was prepared by adding PVDF pellets into the CNT dispersed N-Methyl-2-pyrroli-done (NMP) solution. The flexible CNT/PVDF composite films were investigated by the scanning electron microscopy, which revealed that the CNTs were uniformly dispersed in the PVDF matrix and thickness of the films was approximately 20 jim. Fourier transform infra-red spectra were used to investigate crystal structure of the as-spray-coated CNT/PVDF films, and we found that they revealed extremely large portion of the f3 phase PVDF. The capacitance of the CNT/PVDF films increased by adding CNTs into the PVDF matrix, and finally saturated. However, the resistance didn`t show any saturation effect in the CNT concentration range of 0- 4 wt%. Finally, the resulting nano-generator devices revealed reasonable current output after given mechanical stress.