The composition gradients of 5-500 nm thin NiFe films on Cu, Ru, and NiP substrates, obtained by electrodeposition in stirred plating solutions at pH 3.0 on 8 in wafers, were studied. It was found that the average elemental composition of NiFe, determined by ICP analysis, changes during electrodeposition with steep downturns of Fe-content in composition gradient zone near the substrate interface in the thickness range 5-250 nm depending on the electrode substrate (Cu, Ru, and NiP). The extent of anomalous codeposition achieved at deposit thickness near the substrate (<100 nm) was found to be several times larger than in thicker NiFe films. The partial current densities for metals (Ni, Fe) deposited on Cu-substrates increase during the time of electrodeposition and gives rise to stable values at thickness >250 nm. The partial current density for hydrogen evolution decreases and becomes stable at the thickness>250 nm. The observations related to the experimental results could be explained through a modified Bockris-DrazicDespic (BDD) reduction mechanism. It was found a strong correlation between the dynamics of surface roughening of NiFe films and the anomalous codeposition inside the composition gradient zone. The decrease of Fe-content with time inside the composition gradient zone-which is a special case of anomalous codeposition-was explained through surface roughening of the NiFe films and the surface H + concentration dependent competitive adsorption of FeOH + and NiOH + electroactive species.The electrodeposition of soft magnetic NiFe alloy has been extensively used in the manufacturing of modern recording heads as a reader and writer magnetic shield materials. 1 The soft magnetic NiFe magnetic materials are also used in microelectromechanical (MEMS) devices and numerous applications have been recently reviewed. 2 In particular, the electrodeposition of soft magnetic nanowires and nanoparticles is currently one of the most active research areas in advanced materials. 3,4 The variation of composition of NiFe films, i.e. increase of Fecontent near the substrate at thickness <200 nm was observed more than 50 years ago. 5 The increase of Fe-content in NiFe films affects the following properties: (i) increase of the tensile stress, 6 (ii) increase of positive magnetostriction, 7 and (iii) change of the crystal structure of NiFe films-electrodeposited at the room temperature-from FCC phase (in the range of 10-58 wt% Fe), a mixed FCC/BCC phase (in the range of 59-63 wt% Fe) and BCC phase (in the range of 64-90 wt%). 8 Thereby, the resulting changes profoundly influence the magnetic behavior of NiFe thin films.The composition gradient in the magnetic films at thickness <200 nm, followed by the stabilization of composition during the electrodeposition, is a general phenomena shown that exists in both binary (NiFe; 5,9,10 CoNi; 11 CoFe 12 ) and ternary CoNiFe alloys. 13,14 For the application of thin magnetic film with thickness <200 nm, the composition gradient would be detrimental in controlling of magnetic properti...