A magnetoelectric gradiometer consisting of several Metglas/Pb(Zr,Ti)O 3 sensors with 2D and 3D configurations has been developed. The angular relationship between the ME gradiometer and the magnetic source in different configurations is presented, whose patterns clearly illustrate the magnetic source detection capabilities of our ME gradiometer. At each specific angle, there were unique outputs from the ME sensors, from which we could determine the 2D planar position of the magnetic source. The ME matrix for a 3D magnetic field gradient measurement was also determined. A measurement consisting of eight corner points of a 60 cm × 60 cm × 60 cm cube was performed, where the magnetic source was located in the center of the cube. The experimental data yielded 3D vector outputs representing the distribution of the magnetic flux lines. The results demonstrate that a ME gradiometer has the potential for detection and localization of an unknown spatial magnetic source.