A new kind of magnesium based hydrogen storage alloy with highly developed surface (HDS) was prepared using the technique of mechanical alloying followed by alkali washing in this paper. The phase composition, morphology, hydrogen storage properties and mechanisms of the alloy thus prepared, named HDS Mg-Ni, were further investigated by multiple methods including X-ray diffraction, scanning electron microscope, Sieverts volumetric method and differential scanning calorimeter. The specific surface area, average pore size and pore volume of the alloy are 50.95 m(2) g(-1), 36.2 nm and 0.34 cc respectively. Also, it was discovered that the HDS Mg-Ni powder takes in about 0.65 wt.% of hydrogen even at a low temperature of 323 K, at which the conventional Mg and Mg2Ni materials could not react with H-2. It suggests that the highly developed surface remarkably improves the hydrogen storage properties at low temperatures. Besides, the synergistic effects between the HDS Mg-Ni powder and activated carbon(AC) on the improvement of low-temperature behaviors were discussed. The results showed that the addition of AC further improves the hydrogen capacity and absorption kinetics due to the increased specific surface area, providing easier and more paths for the diffusion of hydrogen into the alloy powder. Copyright (C) 2015, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.