Mechanical alloying of Ti45+xZr38-xNi17 (-4 ≤ x ≤ 16) elemental powder mixtures leads to the formation the amorphous phase, but subsequent annealing at 833 K causes the formation of icosahedral (i) quasicrystal and the Ti2Ni-type crystal phases. The α-Ti phase is also produced in Ti-rich powders after annealing. Both the quasilattice constant of the i-phase and the lattice parameter of the Ti2Ni-type crystal phase decrease monotonically with increasing substituted amount of Ti because of the smaller radius of the Ti atom. The maximum hydrogen concentration in the i-phase in all powder compacts, after electrochemical hydrogenation in a KOH solution, is almost the same, about 63 at% ([H] / [M] ≈ 1.7). The onset temperature of hydrogen desorption is about 570 K (at a heating rate of 5 K/min) for all powders, but the temperature for the maximum hydrogen desorption rate increases with increasing Ti concentration in the powders, suggesting that some hydrogen atoms might be more strongly bound in the quasilattice where the original Zr sites become occupied by Ti atoms.