The multiferroic thin films are promising candidates for applications in magnetic sensors, spintronics, information memory, and other multifunctional devices. In this work, BaTiO3-PVDF/CoFe2O4-PVDF/BaTiO3-PVDF sandwich-structured composites were designed and fabricated by a tape-casting method. The microstructure, dielectric, ferroelectric, magnetic and magnetodielectric properties were systematically investigated. An enhanced ferroelectricity is observed for the maximum polarization (Pmax~1.656 μC/cm2) and the high dielectric constant (εr) of 22 as well as a low dielectric loss for all BaTiO3 filler loading, much better than that of the pure PVDF matrix (εr∼8.26). A recoverable energy density of 0.648 J/cm3 is achieved at an electric field 950 kV/cm, along with a high efficiency (η∼71.0 %). The observed typical magnetic hysteresis loop reveals the presence of long-range ferromagnetic ordering in composites, accompanied by the significant magnetic properties with saturation magnetization (MS~0.507 emu/g), and coercivity (HC~2.3 kOe). Additionally, the response of the dielectric performance under the applied magnetic fields is obvious at RT, i.e., a large negative magnetodielectric coefficient of 2.85 % is obtained at a low magnetic field of 2 kOe, and is up to 6.53 % at 6 kOe for 5 vol% BaTiO3. Ultimately, it is anticipated that this work may provide an efficient method to develop flexible multiferroic composite for multifunctional devices.