Methods of X-ray diffraction analysis, optical metallography, transmission and scanning electron microscopy have been used to study the phase state and structural evolution of binary Al-Fe alloys prepared from a mixture of elemental powders by severe plastic deformation under pressure. The Al-Fe alloys with iron contents ranging from 5 to 50 at. % are produced by a mechanical alloying. The samples are processed up to 30 revolutions. Mechanically alloyed alloys are studied as a function of iron contents. The obtained results demonstrate that super saturated solid solution is formed during the mechanical alloying. It is revealed that the solid solubility of iron in aluminum has been extended up to ~ 1 at. % compared to the maximal value 0.025 at.% at 652°C. It is established that the size of grains depends on the alloying metal content in the alloy and the degree of plastic deformation. After plastic deformation for 30 revolutions, the average grain size in the Al-10 at.% Fe alloy is ~ 5-10 nm. Regions with an amorphous structure are observed in alloys at the iron content > 10 at.%. It has been revealed that the fracture surface stands in a certain causal relation with the iron content in the synthesized alloy: in the alloys Al-5 at.% Fe and Al-10 at.% Fe the fracture surface has traces of ductile fracture, and in the alloys with a higher iron content the fracture is brittle.