Nano-structured Ni80Fe20NCu multilayers were electrodeposited by a newly developed electrodeposition process utilizing a recirculating electrochemical flow reactor. This process, which operates in an inert gas environment, overcomes the limitations of conventional multilayer electrodeposition methods (single and dual bath techniques) by depositing pure magnetic layers without codeposition of the nonmagnetic metal and oxidation of metal interfaces. Structure, corrosion resistance and magnetic properties of electrodeposited NiFe (0 to 100 % Fe) thin film alloys were first investigated. Three different crystal regions, α, mixed α and γ, and γ phases were observed at <50,;50, >50 % Fe in the deposit, respectively. The narrow mixed phase regions was around 50 % Fe compared to 70–80% Fe for bulk alloys. The lattice parameters of electrodeposited alloys exhibited the same trends as bulk alloys. Maximum corrosion resistance was obtained at 50% Fe content in 0.5 M NaCl similar to bulk alloys. The corrosion resistance of the α phase was an order of magnitude less than the γ phase. The magnetoresistance (MR) of electrodeposited NiFe thin film alloys was higher than bulk alloys. Based on these studies, Ni80Fe20/Cu multilayers with individual layer thicknesses ranging from 100 nm to 1.26 μm have been electrodeposited in the recirculating electrochemical flow reactor. The layer thicknesses were precisely controlled by adjusting the amount of charge passed.