Results concerning the preparation and characterization of electrochemically deposited (Fe1-xGax/Fe1-yNiy)n (x=0.1–0.3 at. %; y=0.4–0.8 at. %) multilayered films and nanowires arrays are reported for the first time. The layers have been deposited successively by changing the electrodeposition potential. The combination of Fe1-xGax magnetostrictive material and Fe1-yNiy soft magnetic material shows good magnetic softness (Hc does not exceed 60 G s) and gives novel magnetostrictive behavior caused by the formation of twisted spin structures.