Nanocrystalline CoFe films were fabricated by electrodeposition process for an investigation of the relationship between the alloys’ characteristics and their magnetic properties. The study shows that coating thickness promotes softer magnetic properties of the films, and induces changes of film roughness, preferred orientation and domain pattern. The preferred orientation of the ~1 μm films (thin films) is (110) plane, whereas that of the ~3 μm films (thick films) are (110) and (200) planes. The magnetic domain of the thin films exhibit a stripe-liked pattern, whereas a bubble-liked pattern appears in the thick films. Iron content significantly affects the magnetic properties of the thick films. In this study, the 57.3wt.%Fe thick film has the highest saturation magnetization, and the 80.0wt.%Fe thick film shows the lowest coercivity.