The article deals with the investigation of structure and magnetic properties of plastically deformed Ni51Ti49 alloy. The magnetic hysteresis loops confirm the presence of ferromagnetic properties in the alloy. The transmission electron microscopy (TEM) detects the appearance of lenticular crystals with bending contours which indicate the large distortion of the crystal lattice. The crystal lattice curvature occurs due to the large atom displacement. As a result, icosahedral clusters with the Frank-Kasper (FK) structure can be formed. The spin-polarized density of electron states and the magnetic moments for both non-deformed (near-spherical structure) and deformed (elongated by 5% along the Z-axis) Ni7Ti5 (FK-12), Ni8Ti5 (FK-13), and Ni10Ti6 (FK-16) clusters are calculated for the explanation of possibility of magnetization appearance in Ni51Ti49 alloy. The calculations show the increase in the magnetic moments for the deformed clusters. The calculated spectra demonstrate the high density of electron states near the Fermi level which is a characteristic feature of ferromagnetic alloys.