Magnesium may be the most promising solid-state hydrogen storage material owing to its high storage capacity (7.6 wt%) and highest volumetric density (2 times of liquid H-2). On the other hand, suffers from its sluggish absorption/desorption characteristics. In the present study, the simple/cost-effective hydriding combustion synthesis (HCS) was used to prepare highly-active Mg-based-samples. The preparative parameters of HCS were varied, and its effects on the micro-structural and hydrogen storage properties were determined. The results and its analysis showed that the simple HCS process possesses a multifaceted dependence on a range of experimental factors and affect the final product. The estimated dependence enabled us to explain the combined effect of individual experimental factors on the prepared samples. The Mg-Ni-C sample prepared at 610 degrees C with 6%wt-nano-Ni and 4 wt%-multi-walled-CNTs as reactants, resulted in sample with a surface area as high as 19.01 m(2)/g and a desorption capacity of 5.77 wt%, highlighting the promising characteristics of HCS to prepare highly-active Mg-based-materials. Copyright (C) 2011, Hydrogen Energy Publications, LLC. Published by Elsevier Ltd. All rights reserved.