The influence of ultrafine grains produced by severe plastic deformation technology on the weldability of Fe3Al and Al dissimilar materials was investigated. An ultrafine grain layer was produced on Fe3Al intermetallic compound by surface mechanical attrition treatment. Then the SMATed Fe3Al was diffusion bonded with 1060Al at 550°C for 90 min in the vacuum of 10-3 Pa. The microstructures of surface ultrafine grain layer and transition zone at the interface of SMATed-Fe3Al/Al joint were observed by scanning electron microscopy. The grain size of surface ultrafine grains was characterized by X-ray diffractometry. The elements distribution at the interface and the phase constituents of transition zone were measured by energy disperse spectroscopy. The results showed that a deformed layer about 10-20 μm wide and surface nanocrystallines about 35nm were produced after 15 min surface mechanical attrition. SMATed Fe3Al was well bonded with Al and 11-30 µm wide transition zone formed. The transition zone consisted of FeAl and FeAl3 phases. The surface nanocrystallines helped the atom diffusion and the formation of diffusion bonded joint with rough surface and lower pressure.