In activation of hydrogen storage alloys, the nickel-group metals, especially Pd, act as the catalysts to dissociate hydrogen and turn the alloys into successful hydrogen absorbers. The Laves phase Sc and Zr alloys with Cr Mn as common components exhibit extraordinary hydrogen activation properties matching Pd. Through a cracking mechanism, the bulk samples of these alloys rapidly absorb hydrogen at sub-atmospheric pressures and room-temperature, achieve absorption performance of those Pd surface-modified alloys, meanwhile retaining good reversibility. Among them, the ScCrMn exhibits significantly higher absorption rate than Pd, whereas, the ZrCrMn shows similar absorption kinetics and reversibility to Pd. The shortest initial-activation-time, highest initial-activation-rate and lowest allowed-activation-pressure achieved by ScCrMn are 15 s, -16.6 kPa/s and 0.46 kPa, respectively, in comparison with those of 18 s, 3.2 kPa/s and 0.13 kPa for Pd powder measured under equivalent conditions. The findings and associated magnetization measurements indicate that Cr and Mn upon alloying with certain lower valence metals possess surface electronic structures highly beneficial to hydrogen dissociation. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.