The coexistence of ferroelectric and magnetic order parameters in multiferroic materials opens up a host of new collective properties. In particular, the magnetoelectric (ME) effect namely the induction of electric polarization by a magnetic field or magnetization by an electric field has been widely studied in multiferroics. PVDF is a ferroelectric polymer that has attracted considerable research interest for sensing applications. Compared to traditional ceramic composites, the polymer-ceramic nanocomposites offer inherent advantages, including easy processing, mechanical flexibility and the ability to be moulded into complicated configurations for advanced devices with reduced volume and weight. Additionally, polymer composites generally exhibit superior ME coefficients, attributable to the improved displacement transfer capability of the flexible polymer matrix. In this report, free-standing, flexible and lightweight polymer–ceramic nanocomposite thin films with a fixed weight percentage of ferromagnetic CoFe2O4 nanoparticles have been fabricated using a solution casting technique. The structural, microstructural, and electrical properties of the composite have been characterized by standard experimental techniques. The structural and chemical analyses prove a homogeneous dispersion of the fillers in the microstructure of the composite. The electrical response investigated by impedance spectroscopy reveals the contributions of grains and grain boundaries to the whole impedance of the composites. The ac conductivity as a function of frequency obeys Jonscher’s power law. The improved magnetoelectric properties suggest promising applications in multifunctional devices, including field sensor applications.