The potential use of electrodeposition to synthesize a hybrid magnetostrictive/magnetoelectric layered system is shown in this paper. By appropriately adjusting pH, growth potential, and electrolyte composition, it is possible to achieve thin films in which magnetoelectric oxide GaFeO3 (GFO) is formed in close contact with magnetostrictive metallic FeGa alloy. X-ray diffractometry shows the formation of FeGa as well as GFO and Fe oxides. Electron microscopy observations reveal that GFO mainly segregates in grain boundaries. Samples are ferromagnetic with an isotropic magnetic behavior in the sample plane. Magnetic stripes are observed by magnetic force microscopy and are correlated to Fe3O4. When its segregation is minimal, the absence of stripes can be used to monitor Fe oxide segregation.