We demonstrate a significant control of the polarization response under an applied magnetic field for a magnetoelectric (ME) heterostructure. This structure was comprised of a 2 mu m thick ferroelectric BaTiO3 (BTO) film deposited on flexible ferromagnetic metallic glass foil (25 mu m thick). Au was used as a buffer layer to control BTO growth orientation, and to protect the metallic glass from oxidation. x-ray diffraction and scanning electron microscopy demonstrated the successful growth of well-crystallized BTO films with a high degree of (111) orientation on the amorphous metallic glass foils. Well-defined polarization (P-E) and magnetization (M-H) hysteresis loops confirmed the coexistence of ferroelectric and ferromagnetic properties. A ME voltage coefficient of about similar to 60 mV/cm Oe was measured. (C) 2011 American Institute of Physics. [doi: 10.1063/1.3544352]