A brand-new magnetostrictive/piezoelectric laminated composite is presented using the giant magnetostrictive Terfenol-D, piezoelectric PZT and high-permeability FeCuNbSiB. Since the high-permeability FeCuNbSiB changes the effective magnetic field in the Terfenol-D and the deformed FeCuNbSiB applies a stress to the Terfenol-D in an external magnetic field, thus the saturation magnetostrictive coefficient of Terfenol-D is enhanced, resulting in a higher magnetoelectric voltage output for the composite. Based on the equivalent magnetic charge theory, the effect of the FeCuNbSiB on the effective magnetic field in the Terfenol-D is analyzed, and the magnetostrictive coefficient of Terfenol-D and the theoretical formula of low-frequency magnetoelectric voltage coefficient are derived based on the nonlinear constitutive model of magnetostrictive material and the equivalent circuit method. The analytical results accord with the experiments qualitatively, and the magnetoelectric voltage of the composite is 1.3 times as high as that of the Terfenol-D/PZT-8H (MP) composite. The experimental results indicate that the thickness of FeCuNbSiB has a great influence on magnetoelectric property. The magnetoelectric voltage coefficient increases nearly linearly with the increase of the thickness of FeCuNbSIB until 180μm.