Recently, polymer nanocomposites reinforced with nanoparticles have attracted a lot of attention due to their unique physical and mechanical properties. In this work, poly (vinylidene fluoride)/ nanodiamond particles nanocomposite films were prepared by solution casting method with various nanodiamond particles contents. The samples were investigated by Fourier transform infrared spectroscopy and x-ray diffraction technique. The results revealed an obvious to phase transformation compared to pure PVDF. The most (or the maximum) phase transformation from to phase (>90%) was found for nanocomposite film with8% wt nanodiamond particles. Scanning electron micrographs showed considerable decrease in the size of spherulitic crystal structure of PVDF with adding nanoparticles. The photoluminescence property of nanocomposite films was investigated by photoluminescence spectroscopy and the optical band gap value was calculated from theUV-visible absorption spectra. The results showed that after the incorporation of nanoparticles into PVDF, the value of optical band gap decreased. Thermal stability of samples was studied by thermogravimetric analysis. Due to an increase in the electroactive phase percentage by adding nanoparticles, the resistance of samples to thermal degradation improved. The mechanical properties of samples were investigated by tensile test and hardness measurements. The elastic modulus and hardness of samples were enhanced by adding nanodiamond particles and elongation to fracture decreased.