Fe0.8Ga0.2 films were deposited on bulk single-crystal (0 0 1) 0.69PMN-0.31 PT substrates by DC magnetron sputtering to make magnetoelectric bilayer composites. Films deposited at temperatures below 600 degrees C were X-ray amorphous. Films deposited at temperatures of 600 degrees C and higher exhibited a single-crystal (0 0 1) disordered BCC structure. The crystalline FeGa films demonstrate a 45 degrees twisted cube-on-cube epitaxial relationship with the PMN-PT substrates. Heterostructures with an X-ray amorphous FeGa film exhibited zero magnetcrelectric response. Heterostructures with a 990 nm epitaxial FeGa film exhibited a large inverse magnetcrelectric voltage coefficient of 13.4 (G cm)/V. (C) 2009 Elsevier B.V. All rights reserved.