Lead-free magnetoelectric composite films combining Bi 4 Ti 3 O 12 and CoFe 2 O 4 were synthesized by chemical solution deposition on Pt (100)/Ti/SiO 2 /Si substrate. Morphological and electrical domain structure, ferroelectric, leakage, dielectric, piezoelectric, magnetic and magnetoelectric properties were investigated for Bi 4 Ti 3 O 12 /CoFe 2 O 4 composite films. Well-defined interfaces between Bi 4 Ti 3 O 12 and CoFe 2 O 4 film layers and electrical domain structure were observed. The composite films show the coexistence of ferroelectric and ferromagnetic orders at room temperature. Larger piezoelectric coefficient and magnetization are obtained for the composite films, which is contributed to the magnetoelectric effect since it originates from the interface coupling through mechanical strain transfer. This work presents a feasible way to modulate the magnetoelectric coupling in ferromagnetic/ferroelectric composite films for developing lead-free micro-electro-mechanical system and information storage devices.