Thermomechanical treatment was applied to a binary NiTi alloy in order to improve its functional properties by forming nanocrystalline structure of the alloy. The alloy deformation was obtained by cold rolling combined with transverse movement of the rolls. This technique allowed us to obtain high strain (c ≈ 6) for the relatively large specimens. Subsequently, the samples were annealed in the temperature range 300 -500oC in order to form a nano-, submicro –and/or microcrystalline structure. The evolution of the structure and associated changes of the transformation sequences and functional properties were studied with the use of TEM, X-ray phase analysis, DSC and bend and free recovery ASTM tests. A mixed amorphous/crystalline structure was obtained after severe deformation, the martensitic transformation was completely suppressed in the sample. Annealing at lower temperatures caused formation of nanocrystalline structure that grew to the microcrystalline and finally well-defined polygonized structure in annealed at 500oC specimens.