Magnetic and structural properties of nanocrystalline Fe-Al and Fe-Ni alloys were investigated. Alloys were prepared by the mechanical alloying process. The standard X-ray diffraction, Mössbauer and magnetic studies were carried out on the powder samples. The structural investigations proved that in the low-energy mechanical alloying process of Fe and Al the disordered bcc solid solution was formed up to 50 at.% Al. Alloys were amorphous for Al content between 50 and 90 at.%. The final products of milling exhibited interesting magnetic properties different as compared with microcrystalline alloys. In the case of Fe-Ni alloys the bcc solid solution was formed during high- energy ball milling for the composition with 20 at.% Ni, while above 35 at.% Ni the fcc solid solutions were obtained. All mechanically synthesized Fe-Ni alloys were ferromagnetic and no Invar effect was observed for 35 at.% Ni.