In this study, thin films of Fe 83Ga 17 (a giant magnetostrictive alloy) were grown on single-crystalline n-GaAs (001) and polycrystalline brass substrates via electrochemical synthesis from ferrous and gallium sulfate electrolytes. Extensive structural characterization using microdiffraction, high-resolution ω - 2θ, and rocking-curve analysis revealed that the films grown on GaAs(001) are highly textured with 001 orientation along the substrate normal, and the texture improved further upon annealing at 300°C for 2 h in N 2 environment. On the contrary, films grown on brass substrates exhibited 011 preferred orientation. Rocking-curve analysis done on Fe 83Ga 17/GaAs structures further confirmed that the 001 texture in the Fe 83Ga 17 thin film is a result of epitaxial nucleation and growth. The non-linear current-voltage plot obtained for the Fe-Ga/GaAs Schottky contacts was characteristic of tunneling injection, and showed improved behavior with annealing. Thus, this study demonstrates the feasibility of fabricating spintronic devices that incorporate highly magnetostrictive Fe (1-x))Ga x thin films grown epitaxially via electrochemistry.