A novel laminate composite of FeCuNbSiB/FeNi /PZT is proposed, where FeCuNbSiB has a permeability of around 100000, which is much larger than that of FeNi. The high-permeability FeCuNbSiB was laminated with piezomagnetic FeNi rather than attached to its ends. It is expected that the effect produced by the high permeability will act on the whole of the piezomagnetic layer. While a FeNi layer was laminated with a FeCuNbSiB layer, the strong demagnetization produced by the latter was expected to be imposed on the FeNi layer as well as the applied fields. The distribution of applied fields was altered by the high-permeability material (both bias and ac field) and the field variation positively contributed to the ME effect in piezomagnetic/piezoelectric composites. Thus the ME voltage coefficient along with the field sensitivity were improved.