The structural and the magnetic properties of nanocrystalline and amorphous Fe55Mn10Al35 alloys prepared by the mechanical alloying process are studied as functions of the milling time varying from 1 hr to 48 hrs. Structural analyses based on X-ray diffraction (XRD) and extended X-ray absorption fine structure spectroscopy (EXAFS) reveal that the alloying process took place after 12-hr milling. Nanocrystalline alloys are found until 24-hrs milling, and an amorphous phase afterward. Concerning the magnetic behavior, the data obtained from a vibrating sample magnetometer show that both the magnetization saturation (Ms) and the coercivity (Hc) are dependent strongly on the milling time and the crystallite size. By adjusting the milling time, both appropriate structural transformation and magnetization values are obtained.