Abstract: The influence of the electrodeposition potential on the compositional, magnetic, and microstructural properties of CoFe alloy thin films grown on a Cu sputtered silicon substrate was studied. Grazing incidence X-ray diffraction results indicate a diffraction peak at 2θ ≈ 45° related to (110) plane of a body-centered cubic structure of CoFe alloy. Field emission scanning electron microscopy images reveal densely packed uniform nano-granular morphology in all films. Energy-dispersive X-ray spectroscopy results indicate a variation in CoFe alloy film composition while varying the deposition potential, attributed to anomalous co-deposition. The magnetic hysteresis loop measurement shows films are having an easy magnetic direction oriented along in-plane, with high saturation and low coercivity. Surface and microscopic magnetization measurements prove that the deposition potential modifies the film roughness and influences the magnetic domain formation. © 2020, Allerton Press, Inc.