Magnetic/ferroelectric multilayer thin films using PbZr0.52Ti0.48O3 (PZT) and two different magnetic materials, i.e., Terfenol-D and CuFe2O4 (CuFO) layers, were fabricated, and their magnetoelectric (ME) coupling behavior was investigated. The PZT layer was first coated onto Pt/Ti/SiO2/Si substrate by sol-gel spin coating method. Pt layer, which served as an electrode and a diffusion barrier, was grown on the PZT layer by using the ion-beam sputtering method. The ME voltage coefficients were calculated from the ME voltage data measured utilizing a magnetoelectric test system. The Terfenol-D/Pt/PZT films were found to show a higher in-plane ME voltage coefficient than that the CuFO/Pt/PZT films due primarily to the higher magnetostriction coefficient of Terfenol-D.