Hydrogen separation alloys V85Ti10Y5 and V85Ti10Cu5 were prepared by high vacuum non-consumable arc melting furnace. The effects of the addition of Y and Cu elements on the hydrogen permeability, hydrogen solubility and hydrogen brittleness resistance of the alloy were investigated by SEM, TEM, XRD, hydrogen permeability test, PCT hydrogen absorption test and constant pressure slow cooling test. The results show that the as-cast V85Ti10Y5 and V85Ti10Cu5 alloys are both composed of V-matrix and the second phase, but the second phase of the former is dispersively distributed Y-rich particles, while the latter is a Cu-Ti intermetallic compound precipitated in the grain and distributed continuously along the grain boundary. The formation of Y2O3 in V85Ti10Y5 alloy and the hydrogen-repulsive action of some solid solution Cu in V85Ti10Cu5 alloy and the formation of Cu2Ti reduce the solid solution amount of Ti in V, and then reduce the concentration of hydrogen in the alloy, reduce the internal stress generated by hydrogen solution, improve the anti-hydrogen brittleness. The V85Ti10Y5 and V85Ti10Cu5 alloys showed excellent anti-hydrogen embrittlement properties without hydrogen embrittlement during slow cooling. Moreover, the hydrogen permeability at 673 K is 0.139×10-6 mol H2 m-1 s-1 Pa0.5 and 0.174×10-6 mol H2 m-1 s-1 Pa0.5, which is 5.5 and 6.9 times of Pd77Ag23. Compared with commercial palladium alloys, they all show higher permeability.