The effects of microstructure on hydrogen absorption in FeTi are reported. Powders of FeTi with different microstructures (nanocrystalline and amorphous) were prepared by high-energy ball-milling. FeTi powders were also modified with small amounts (less than 1 wt %) of palladium catalyst to eliminate activation. Enhancements in hydrogen absorption for both nanocrystalline and amorphous FeTi powders were observed.