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Magnetoelectric (ME) devices based on Fe-Ga/AlN/Mo thin films deposited on Si(100) substrates were prepared by magnetron sputtering. The cantilever device possessed a high magnetoelectric coefficient of 167.7 V/cm·Oe at its resonance frequency and exhibited anisotropic properties. More importantly, the magnetoelectric coefficient changed with the out-of-plane space angle, from 15 to 167.7 V/cm·Oe. After annealing under a 500-Oe magnetic field, the magnetic domains of the thin film partly remained in the field direction. Moreover, the anisotropic properties of the ME device significantly improved; the ME coefficient increased by 30% to 218 V/cm·Oe and became more sensitive to the in-plane angle. Thus, the ME device proposed in this work can be used to detect changes in spatial angles.