Nanocomposites comprising (V2O5)x. (Mn0.4Fe2.6O4)(2−x), where x = [0.2, 0.4, 0.6, 0.8, and 1], were successfully synthesized by milling each single phase of V2O5 and Mn0.4Fe2.6O4 nanostructured samples. We studied the structure and morphology of the prepared samples through X-ray diffraction and scanning electron microscopy. UV–Vis. spectrum analysis was used to study the optical characteristics. As an attempt to improve the optical and nonlinear optical properties of the PVDF blend, the prepared nanocomposites were used as nanofillers for the poly (vinylidene fluoride) (PVDF) polymer. Optical and nonlinear optical properties of the PVDF polymer were tuned using (V2O5)x. (Mn0.4Fe2.6O4)(2−x), where x = [0.2, 0.4, 0.6, 0.8, and 1] nanocomposite. The obtained results showed a tunable spectrum, absorption, refractive index, and dielectric constant at wavelengths ranging from 200 to 800 nm. However, the results showed that the (V2O5)0.6. (Mn0.4Fe2.6O4)1.4, sample was the best for obtaining the lowest transmittance percentage and bandgap energy. The nonlinear optical properties and Kerr effect (quadratic electro-optic effect) showed a significant response, which can be tuned in the range from 200 to 1200 nm of wavelength using the investigated samples. Finally, incorporating (V2O5)x. (Mn0.4Fe2.6O4)(2−x), where x = [0.2, 0.4, 0.6, 0.8, and 1], nanoparticles in the PVDF polymer improved the hydrophilic behavior of the PVDF films. This study suggests a promising nanocomposite material for tunable optoelectronics and useful polymer membranes. [ABSTRACT FROM AUTHOR]