Al–Fe alloys with concentrations of iron of up to 50 at % have been produced from elemental powders using severe plastic deformation by high-pressure torsion. The synthesized alloys were studied using X-ray diffraction structural analysis and transmission and scanning electron microscopy, as well as microhardness measurements. It has been found that the grain size depends on both the degree of plastic deformation and the concentration of iron in the alloy. Plastic deformation by high-pressure torsion results in the mutual dissolution of iron and aluminum atoms. At room temperature, the solubility of iron in aluminum reaches ~1 at %. The dissolution of aluminum in the iron lattice leads to the formation of a disordered FeAl solid solution. With an increase in the concentration of iron in the alloy, its microhardness monotonically rises to a value of 3.4 GPa.