Magnetoelectric (ME) Ni/Pb(Zr0.52Ti0.48)O3 bilayers have been successfully prepared by hydrothermal method using Ti as buffer layer. The hydrothermal mechanism of PZT thin film deposited onto Ni layer has been discussed. The structure and ferroelectric properties of the deposited PZT thin films are characterized by X-ray diffraction and ferroelectric testing. The ME voltage coefficient of the Ni /PZT bilayers gradually decreases as the thickness of buffer layer increases because the interface coupling of the Ni /PZT layers gradually decreases. The large ME coefficient makes these Ni /PZT bilayers possible for applications in multifunctional devices such as electromagnetic sensor, transducers and microwave devices.