Flexible CoFe2O4/PVDF (CFO/PVDF) composite films were prepared using the casting method, and the effects of CFO particle concentrations on the physical phase, structure, and magnetoelectric properties were investigated. The results demonstrate that the strip CFO particles are successfully incorporated into the PVDF matrix and dispersed uniformly. The incorporation of an appropriate quantity of CFO particles is found to enhance the beta-phase content. As the CFO particle concentrations increase, the magnetic properties change linearly, while the dielectric and ferroelectric properties demonstrate excellent performance. When the CFO particle concentration is 10 %, the dielectric constant and residual polarization intensity reach their maximum values of 64.72 and 1.1617 mu C/cm2, respectively. The observed enhancement of ferroelectric properties following the application of a magnetic field indicates that the composite films exhibit significant magnetoelectric coupling effects. The magnetoelectric coupling coefficient (alpha ME) reaches its maximum value of 52.06 V/(cm center dot Oe) when the CFO particle concentration is 20 %. Furthermore, the tensile test demonstrates that the composite films exhibit excellent flexibility. These findings suggest that flexible composite films have extensive potential for applications in flexible sensors and energy harvesting.