The Fe3Al-based intermetallics were prepared by mechanical alloying and spark plasma sintering (SPS), and the influence of milling time on the properties of materials was investigated. The phase identification was investigated by X-ray, and the surface morphology and fractography were observed by scanning electron microscope (SEM). The mechanical properties such as bending strength, strain, and microhardness were tested. The results show that Fe reacts with Al completely to form Fe3Al during short SPS processing time. The relative densities of the sintered samples were nearly 100%. The mechanical properties of the sintered samples can be improved along with the milling time. The representative values are the bend strength of 1327 MPa and the microhardness of 434.