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As a floppy alloy, the silicon steel with a content of Si of 6.5% has been paid much attention due to its maximum magnetic induction and minimum iron loss. However, the manufacture has been limited largely by conventional technics. By comparison, the silicon steel with a lower silicon content of 0.1%-4.0%, which was manufactured by conventional technics, also has a limited application. In this work, Molten Salts Electrodeposition has been employed to produce Fe-Si alloy. Technological parameters including influence of Molten Salts Electrodeposition technic in aggradation layer appearance and distribution of silicon content along with thickness. The results also show that the size of superficial particles on deposit layer increased gradually, the thickness of deposit layer was proportional to the current density on the deposit layer of Fe-Si.