Multiferroic materials (MFM) have drawn substantial attention for developing smart magnetodielectric devices. Herein, cobalt ferrite CoFe2O4 (CFO) was synthesized by a glycine–nitrate sol-gel auto-combustion route and, PVDF-based particulate composite films embedded with CFO have been developed. A comprehensive investigation evaluated the effects of magnetostriction, initiated from the embedded CFO phase, on magnetodielectric characteristics of composite films. The structural, electrical, magnetostrictive and magnetodielectric properties were investigated. The embedded CFO particulate endows PVDF matrix at a higher β–phase forming ability, which enhances the ferroelectricity with a polarisation (Pmax∼1.09 μC/cm2@ 850 kV/cm), a higher dielectric constant (εr∼12.33) and lower dielectric loss. The typical magnetic hysteresis loop was obtained with saturation magnetization (MS∼4.96 emu/g) and coercivity (HC∼1.49 kOe), revealing the ferromagnetic ordering in composite films. The response of the magnetodielectric (MD) is observed at room temperature, that is, a large negative MD coefficient ∼2.1 % @ Hcr∼5.0 kOe is achieved for Co0.9Fe2.1O4/PVDF composite films, while MD∼0.65 %@ Hcr∼1.0 kOe is obtained for Co1.1Fe1.9O4/PVDF films, accompanied by a maximum MD∼4.35 % at resonance frequency. The variation in the MD performance reveals a close correlation to the modulated magnetostriction, such as the magnetocrystalline anisotropy, field-induced coefficient and magnetostrictive susceptibility, indicating the strain-mediated coupling MD effect. The multiferroic properties in CoxFe3–xO4/PVDF composites have potential for magneto-dielectric sensing applications. Furthermore, this work would be exploited to understand MD coupling mechanism and develop MFM for multifunctional devices.