We report the synthesis of the Fe 100−x Co x (x = 55, 50, 45) alloys by two ways consisting in high energy ball milling and polyol process. A structural and morphological study of all samples has been undertaken by X-ray diffraction (XRD) using the Rietveld method, by scanning electron microscopy (SEM), and by transmission electron microscopy (MET). The size and crystallinity of the particles was found to depend on the synthesis method. The magnetic properties and the DOS calculation have been also investigated. It has been found that both were remarkably dependent on the Co/Fe molar ratio. It has been observed that the best magnetic properties was obtained for the sample x = 45 prepared by the polyol process where M s = 235 emu/g and H c = 93 Oe. We have shown also that the random local anisotropy field H r and the local anisotropy K L decrease with increasing Co content.