Ni-Fe alloy/ZnO nanorod composites were fabricated and the magnetoelectric effect was demonstrated. The ZnO and Ni-Fe alloy serve as the piezoelectric phase and the magnetostrictive phase in the nanocomposite, respectively. Since the nanorod structure possesses the inherent nature of a large surface-to-volume ratio, it greatly enhances the interplay between the piezoelectric and magnetostrictive coupling. Besides, the substrate clamping effect can be avoided. Our newly devised composite therefore provides a different species for magnetoelectric applications. It is interesting that the magnetoelectric voltage coefficient determined by the direct measurement method can reach a value as high as 0.48 mV cm(-1) Oe(-1).