The optical properties of polyvinylidene fluoride (PVDF) polymer nanocomposite films incorporating SrTiO3/carbon nanotubes (CNTs) as nanofillers are investigated. PVDF/SrTiO3/CNTs films were prepared by the solution casting technique. X-ray diffraction (XRD), Fourier-transform infrared spectroscopy (FTIR), and scanning electron microscopy (SEM) analyses confirmed the incorporation of SrTiO3/CNTs into the PVDF matrix. The addition of nanofillers influenced the crystalline structure, morphology, and optical properties of the films. SEM images showed spherulite morphology, which is a spherical aggregate of crystalline polymer chains. The addition of a SrTiO3/CNTs nanofiller modified the polymer’s electronic structure, causing a variation in the energy gap. The addition of SrTiO3/CNTs at 0.1 wt% increased the band gap, refractive index, and nonlinear optical properties of the PVDF films. These improvements indicate the potential of these nanocomposite films in optoelectronic applications such as solar cells, image sensors, and organic light-emitting diodes.