Incorporation of different types of nanofillers in the PVDF poly(vinylidene difluoride) matrix exhibits promising dielectric, magnetic, piezo, pyro, and ferroelectric properties for various applications. Hence a novel nanocomposite has been developed by using PVDF and cobalt ferrite (CFO) (CoFe 2 O 4 ) with different particle size of CFO for dielectric applications. The nanocomposite has been characterized by the X-ray diffraction pattern, atomic force microscopy, transmission electron microscopy, fourier transform infrared spectroscopy, field emission-scanning electron microscopy), and dielectric measurements. The space charge effect at the PVDF and CFO interfaces offers the interfacial polarization in nanocomposite, which contribute to tune the dielectric response of nanocomposite along with low dielectric loss. The filler size has been optimized to have better formation of polar β phase in PVDF along with high dielectric properties. The dielectric constant in nanocomposite has increased three times compare to that of PVDF. The 20 ± 1 nm size (CFO) filler in PVDF matrix exhibits optimized dielectric properties.