Abstract The physical-mechanical properties of the Ti-Ta based surface alloy with thickness up to ∼2 μm fabricated through the multiple (up to 20 cycles) alternation of magnetron deposition of Ti70Ta30 (at.%) thin (50 nm) films and their liquid-phase mixing with the NiTi substrate by microsecond low-energy, high current pulsed electron beam (LEHCPEB: ≤15 keV, ∼2 J/cm2) are presented. Two types of NiTi substrates (differing in the methods of melting alloys) were pretreated with LEHCPEB to improve the adhesion of thin-film coating and to protect it from local delimitation because of the surface cratering under pulsed melting. The methods used in the research include nanoindentation, transmission electron microscopy, and depth profile analysis of nanohardness, Vickers hardness, elastic modulus, depth recovery ratio, and plasticity characteristic as a function of indentation depth. For comparison, similar measurements were carried out with NiTi substrates in the initial state and after LEHCPEB pretreatment, as well as on “Ti70Ta30(1 μm) coating/NiTi substrate” system. It was shown that the upper surface layer in both NiTi substrates is the same in properties after LEHCPEB pretreatment. Our data suggest that the type of multilayer surface structure correlates with its physical-mechanical properties. For NiTi with the Ti-Ta based surface alloy ∼1 μm thick, the highest elasticity falls on the upper submicrocrystalline layer measuring ∼0.2 μm and consisting of two Ti-Ta based phases: α′′ martensite (a = 0.475 nm, b = 0.323 nm, c = 0.464 nm) and β austenite (a = 0.327 nm). Beneath the upper layer there is an amorphous sublayer followed by underlayers with coarse (>20 nm) and fine (