A nanocrystallines surface layer was produced in Fe3Al intermetallic compound by surface mechanical attrition treatment (SMAT). The microstructure of deformed layer, phase structure and morphology of surface nanocrystallines were characterized through optical microscopy, X-ray diffractometry, transmission electronic microscopy and high resolution electronic microscopy. The results show that a deformed layer about 11μm wide is produced after 10min surface mechanical attrition. The grains on the top surface of Fe3Al are refined to nanocrystallines and the grain size of nanocrystallines is about 35nm. High density dislocations collect on the boundaries of grains. The formation of nanocrystallines is controlled by grain subdivision mechanism.