Magnetoelectric Tb0.3Dy0.7Fe1.92(Terfenol-D)/PbZr x Ti1−x O3(PZT) bilayer thin films were deposited on (111)-oriented Pt/Ti/SiO2/Si< 100 > substrates. The PZT layers with different compositions (x = 0.3 and 0.52) were grown on the substrates by using the sol-gel method. Terfenol-D layers were deposited on the PZT-film-coated substrate by ion beam sputtering at room temperature with a dot-type patterned metal shadow mask. The structural characteristics and the ferroelectric, ferromagnetic and magnetoelectric(ME) properties of the Terfenol-D/PZT bilayer thin films were investigated. In our results, the maximum remnant polarization, 2P r were ∼60 µC/cm2 for Terfenol-D/PZT(30/70) (Zr/Ti ratio = 30/70). The magnetization and the ME voltage coefficients were identical regardless of the Zr/Ti composition of PZT. The ME voltage coefficients of the films were over 400 mV/cm·Oe, which were about 4 times higher than the values reported for other bilayer structures.