Elemental Ti and Fe powders were mechanically alloyed using a high-energy ball mill and a conventional ball mill in an argon atmosphere. The morphology, structure, and hydriding behavior of the resultant powders were compared. The powders milled for 100h using a conventional ball mill consisted of Ti and Fe phases together with TiFe phase. On the other hand, those milled for 100 h using a high-energy ball mill consisted mostly of the TiFe phase together with a small amount of Ti and amorphous phases. The mechanically alloyed powders were easily absorbed hydrogen after one step activation with heating at 723 K in vacuum and subsequent hydrogenation at room temperature. The characteristics of the pressure-composition-temperature (PCT) curve were deeply dependent on the amounts of Ti and TiFe phases in the mechanically alloyed powders. The powders milled for 100 h using a high-energy ball mill had a lower plateau pressure than those milled for 100 h using a conventional ball mill. These mechanically alloyed Ti-Fe powders had a lower plateau pressure than the fully activated Ti-Fe alloy counterparts.