In this research, piezoelectric polymer nanocomposite films were produced through solution mixing of laser-synthesized Au nanoparticles in poly (vinylidene fluoride) (PVDF) matrix. Synthetization of Au nanoparticles was carried out by laser ablation in N-methyle-2-pyrrolidene (NMP), and then it was added to PVDF: NMP solution with three different concentrations. Fourier transformed infrared spectroscopy (FTIR) and X-ray diffraction (XRD) were carried out in order to study the crystalline structure of the nanocomposite films. Results revealed that a remakable change in crystalline polymorph of PVDF has occurred by embedding Au nanoparticles into the polymer matrix. The polar phase fraction was greatly improved by increasing the loading content of Au nanoparticle. Thermogravimetric analysis (TGA) showed that the nanocomposite films are more resistant to high temperature and thermal degradation. An increment in dielectric constant was noticed by increasing the concentration of Au nanoparticles through capacitance, inductance, and resistance (LCR) measurement. Moreover, the mechanical properties of nanocomposites were numerically anticipated by a finite element based micromechanical model. The results reveal an enhancement in both tensile and shear moduli.