Using pulsed laser deposition, multiferroic La2/3Sr1/3MnO3(LSMO)/BaTiO3(BTO) composite films are deposited on LaAlO3 (LAO)(001) substrate. X-ray diffraction results show that LSMO and BTO films exhibit only (001) orientation. Film smoothness is verified by their low root-mean-square surface roughness values as 1.4 nm from atomic force microscope study. The magnetic and the electric properties of these composite films are investigated. Furthermore, the variations of resistivity and metal-insulator transition temperature TMI of LSMO, induced by the external electric field, are studied. The resisitivity is reduced while the TMI is enhanced for hole accumulation state which is induced by negative electric field across BTO layer. In contrast, the resistivity is enhanced while the TMI is reduced for hole depletion state, which shows coupling between magnetic and electric order parameters, i.e., there is a magnetoelectric effect induced by electric field.