Perovskites BaTi1-zFezO3+δ with doping level from 0.005 to 0.02 have been synthesized with sol-gol method. The X-ray diffraction shows that the doped perovskites retain the original tetragonal structure. Defferential thermal analysis demonstrates that both the transformation temperature of ferroelectric to paraelectric and the latent heat of the transformation decrease with increasing doping level. Bilayer composites BaTi1-zFezO3+δ-Tb1-xDyxFe2-y bilayer composites havebeen fabricated after the piezoelectrics being poled and their magnetoelectric effect has been investigated using a bias magnetic field and an ac magnetic field of 100Hz. The experimental result shows that the transverse magnetoelectric voltage coefficient of the bilayer composites can reach a maximum at doping level of 1.5%. The value of the maximum is 1788mV/A under a bias magnetic field of 60kA/m at room temperature. The analysis of magnetoelectric spectroscopy also shows a higher resonance peak and a higher resonance frequency for the sample containing BaTi0.985Fe0.015O3+δ， suggesting a higher piezoelectric coefficient in the doped BaTiO3 and some difference in interfacial coupling coefficients in the bilayer composites containing the doped samples， respectively.