Magnetoelectric (ME) Ni/Pb(Zr0.52Ti0.48)O-3 bilayers have been prepared by hydrothermal method. The structure and ferroelectric properties of the Pb(Zr0.52Ti0.48)O-3 (PZT) thin films prepared at various hydrothermal temperatures are characterized by X-ray diffraction and ferroelectric testing. With the hydrothermal temperature increasing the grain size of the PZT thin films gradually decreases leading to a gradual increase of the coercive field and a decrease of the remnant polarization of the Ni/PZT bilayers. The ME voltage coefficient of the Ni/PZT bilayers gradually decreases as hydrothermal temperature increases. The large ME coefficient makes these Ni/PZT bilayers possible for applications in multifunctional devices such as electromagnetic sensor, transducers and microwave devices. (C) 2012 Elsevier B.V. All rights reserved.