The desorption of hydrogen from a novel material, a Ti45Zr38Ni17‐H quasicrystal, was observed using high‐temperature powder x‐ray diffraction, demonstrating the potential utility of Ti‐based quasicrystals in place of crystalline or amorphous hydrides for hydrogen storage applications. The maximum observed change in hydrogen concentration was from 61 at. %, corresponding to a hydrogen‐to‐metal ratio (H/M) of 1.54, at 91 °C to less than 2.5 at. % (H/M=0.025) at 620 °C. The onset temperature of desorption is below 350 °C. Surface oxidation was found to promote the formation of crystalline hydride phases. Highly oxidized samples transformed to a mixture of the C14 Laves and C15 Laves crystalline hydrides, and the Ti2Ni phase. When the oxidation was less severe, a reversible transformation between the quasicrystal and crystalline hydride phases was clearly observed, demonstrating the stability of the Ti45Zr38Ni17 quasicrystal at very low hydrogen concentrations, and temperatures as high as 661 °C. This is the first evidence for a stable Ti‐based quasicrystal and for reversible hydrogen storage in a quasicrystalline phase. © 1996 American Institute of Physics.