Using　pulsed　laser　deposition　technique,　the　multiferroic　BaTiO3/La2/3Sr1/3MnO3　composite　bilayer　films　were　epitaxially　prepared　on　(001)　oriented　LaAlO3　single　crystal　substrate.　The　measurements　of　electric　and　magnetic　properties　showed　that　the　composite　structure　possessed　superior　ferromagnetic　and　ferroelectric　properties,　its　relative　dielectric　constant　and　ferromagnetic　curie　temperature　were　263　and　317　K,　respectively.　The　magnetoelectric　voltage　coefficient　for　the　bilayer　films　at　room　temperature　was　around　176　mV/A,　which　was　at　least　one　order　of　magnitude　higher　than　the　previous　reported　in　the　same　structures.　The　corresponding　interface　coupling　parameter　k　was　about　0.68,　which　indicated　a　better　interface　coupling　between　ferromagnetic　and　ferroelectric　layers.