The characteristics of X-ray Diffraction (XRD), Current (I)-Voltage (V), and the Polarization-Electric field (P-E) on the BiFeO3 (BFO), BaTiO3 (BTO), and our proposed Multi-Layer (ML) BiFeO3/BaTiO3 (BFO/BTO) samples are studied systemically. The influence of these films with and without different external Magnetic (Mex.) inputs is also investigated. Our proposed multi-ferroic ML BFO/BTO sample has a lower tunneling current (Jg) (~5 × 103 times) and a stronger magneto-electric effect (an ~25 times higher value of the change of saturated polarization Ps with the Mex. inputs than the pure multi-ferroic BFO sample. The material properties for ML BFO/BTO samples can be optimized with the combination of the advantages of BFO and BTO thin films. The stronger magneto-electric effect in our proposed ML samples can have many applications such as magnetic sensors, magnetic electric devices, and logic Magneto-Electric Spin–Orbit (MESO) devices.