The electron-beam cycling additive technique was proposed for the formation of shape memory Ti-Ta coatings on titanium substrate. On a commercially pure Ti plate, Ta film with a thickness of about 4 μm was deposited by direct current (DC) magnetron sputtering. The sample was then subjected to an electron-beam surface alloying by a scanning electron beam. On the already-formed Ti-Ta surface alloy, a Ta coating with the same thickness was further deposited and the specimen was again subjected to electron-beam alloying for the second cycle. The same procedure was repeated for the third cycle. The structure obtained after each cycle Ti-Ta coatings was studied by X-ray Diffraction (XRD), Scanning Electron Microscopy (SEM), and Energy-dispersive X-ray spectroscopy (EDX). The Young’s modulus, hardness, and shape memory effect (SME) were studied by nanoindentation experiments. The results showed that the thickness of the Ti-Ta coatings is about 50 μm in all cases, where the Ta content increases after each technological cycle. It was found that the obtained phase composition is in the form of a double-phase structure of α’ martensitic and β phases, where the highest amount of beta is registered in the case of the Ti-Ta coating obtained after the third cycle. The results obtained for the Young’s modulus and hardness showed that both mechanical characteristics decrease significantly after each cycle. Additionally, the elastic depth recovery ratio increases with an increase in the number of cycles.