A nanostructured surface layer was successfully performed on a biomedical beta-type TiNbZrFe alloy by surface mechanical attrition treatment (SMAT). The results reveal that the surface layer along the depth from treated surface to strain-free matrix could be divided into an outer nanocrystalline layer (0-30 mu m), a high-density dislocation region (30-200 mu m) and an inner region with low-density dislocations and twins (200-700 mu m) when the surface was treated for 60 min. The microhardness of the surface layer is enhanced and increases with increasing treatment time. Although the {1 1 2} (1 1 1) twin coordinates the deformations with dislocations, this coordination only occurs in the low strain area and cannot affect the nanocrystalline formation. The self-nanocrystallization of TiNbZrFe alloy is mainly attributed to dislocation movements. First, the dislocations start to move and easily form dislocation bands along certain crystal directions; then, multiple slips of dislocations gradually form dislocation tangles; after that, high-density dislocation tangles increases, which divides primary grains into many small domain areas. As high strain energies accumulate on the interfaces among these areas, the lattice rotation can be driven between the adjacent small domain areas, finally resulting in a large number of nanocrystalline regions with low or large angle grain boundaries. (C) 2015 Elsevier B.V. All rights reserved.