Chromium doped BaTiO3 was synthesized with sol-gel technique. The Cr-doped BaTiO3 was still Ill the structure of tetragonal perovskite by X-ray diffraction, and its transformation point of ferroelectric to para-electric as well as the latent heat of the transformation were observed a little less than those of pure BaTiO3, respectively, by the tests of differential scanning calorimetry. Layered composites Tb1-xDyxFe2-y and BaT1-zCrzO3-delta were fabricated by bonding the discs of the doped BaTiO3 and rare earth alloy Tb1-xDyxFe2-y The magnetoelectric (ME) effect of the layered samples was investigated. The transverse ME voltage coefficient for the bilayer Tb1-xDyxFe2-y-BaTi1-zCrzO3-delta and the trilayer Tb1-xDyxFe2-y-BaTi1-zCrzO3-delta-Tb1-xDyxFe2-y reach 732.5 and 2753mV/A, respectively, under a bias magnetic field 28kA/nm at room temperature, which are about 54% and 56% larger than those for the bilayer and trilayer composed by pure BaTiO3, respectively. Since Cr-doped BaTiO3 does not contain injurants, such as lead and zirconium, it can replace lead zirconium titanite as a "green" piezoelectric material for ME composites.