The connection of Ti–H by ATAT, USPEX codes with QE and VASP interfaces is investigated in the work. Predictive estimates revealed a number of stable and geometrically optimized hydrides with different atomic compositions: Ti6H2, Ti5H3, Ti5H2, Ti4H3, Ti3H5 of a simple triclinic group and highly symmetrical TiH2, Ti2H2, Ti6H2, Ti3H5 alloys. The stability of hydrides was evaluated by first principles calculations and by the convex hull method. Model estimates of mechanical characteristics have shown that hydrides with low mass density are high-strength compounds. The detected hydrides can be included in the reference database of Ti–H compounds. The possibility of obtaining alloys based on Ti–Al with additions of Sc, Y, Dy, Ho by “Hydride technologyˮ is considered. The formation of a lamellar structure upon the introduction of 2 at.% Sc, Y into Ti–50Al (at.%) was found. When 2 at.% Dy, Ho is added to Ti–50Al (at.%), isotype compounds Y6Ti4Al43, Dy6Ti4Al43, Ho6Ti4Al43 are formed. The values of microhardness and electrical resistance are given.