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The effect of a promising method of performing a thermomechanical treatment which provides the nanocrystalline structure formation in bulk NiTi shape memory alloy samples and a corresponding improvement to their properties was studied in the present work. The bi-axial severe plastic deformation of Ti-50.7at.%Ni alloy was carried out on the MaxStrain module of the Gleeble system at 350 and 330 °C with accumulated true strains of e = 6.6-9.5. The obtained structure and its mechanical and functional properties and martensitic transformations were studied using DSC, X-ray diffractometry, and TEM. A nanocrystalline structure with a grain/subgrain size of below 80 nm was formed in bulk nickel-enriched NiTi alloy after the MaxStrain deformation at 330 °C with e = 9.5. The application of MaxStrain leads to the formation of a nanocrystalline structure that is characterized by the appearance of a nano-sized grains and subgrains with equiaxed and elongated shapes and a high free dislocation density. After the MaxStrain deformation at 330 °C with e = 9.5 was performed, the completely nanocrystalline structure with the grain/subgrain size of below 80 nm was formed in bulk nickel-enriched NiTi alloy for the first time. The resulting structure provides a total recoverable strain of 12%, which exceeds the highest values that have been reported for bulk nickel-enriched NiTi samples.