The epitaxial La 0.7 Sr 0.3 MnO 3 /BaTiO 3 (LSMO/BTO) bilayer films with various volume fraction ν of ferroelectric (FE) phase (BTO) are fabricated on (001) oriented LaAlO 3 substrate. The value of ν is regulated by changing the thickness of LSMO film, and fixing the thickness of BTO film. The value of ν is demonstrated to play a key role in determining the interface magnetoelectric (ME) coupling coefficient (k) of the LSMO/BTO bilayers, i.e. a lower value of ν leads to a lower value of k. Furthermore, as ν is 0.91, experimental value of the ME voltage coefficient α E is higher than its calculated value, which indicates that the main ME coupling mechanism have evolved from strain-mediated to charge-mediated. This result can provide an available method for the design of multiferroic composite bilayer films with adjustable ME coupling mechanism by optimizing the volume fraction of FE phase.