In this work, mainly a solid solution of Fe dissolved in Al matrix was prepared by the high energy ball milling technique from a stoichiometric mixture of high purity powders of Fe and Al. The ball milling process was performed by using a fixed ball weight/sample weight ratio of 10:1. The particle size increased significantly from 4 to 6 h of milling, but after that time, decreased to the end of milling time (10h). According to X-ray diffraction analysis, a solid solution of Fe in Al (α-Al) begun to form at the fourth hour of milling. The crystallite size corresponding to the solid solution (α-Al) was decreased as the milling time advanced. Also, the calculated lattice parameter displayed a tendency to decrease as the milling time elapsed. The transmission electron microscopy (TEM) analysis revealed the precipitation of the Al5Fe2 and Al13Fe4 phases in the Al matrix.