Icosahedral quasicrystalline phase (I-phase) formed in a number of Ti-based alloys, and that the I-phase was well ordered and thermodynamically stable in the Ti-based alloy. Further, studies on the physical/chemical properties have received much attention. It was important from scientific and technological point to study the preparation and hydrogen storage property of the alloys. Recently we have prepared single I-phase Ti45Zr35Ni17Cu3 powder and investigated their hydrogen storage property. Here, we reviewed the research results and proposed the research of Ti/Zr-based I-phase as hydrogen storage material.