The objective of the present work was to investigate the possibility of improving the hydrogen-storage capacity of mesoporous MCM-41 containing nickel (Ni) oxides (Ni/MCM-41). The MCM-41 and Nil MCM-41 were prepared using a hydrothermal process as a function of Ni content (2, 5, and 10 wt.% in the MCM-41) The surface functional groups of the Ni/MCM-41 were identified by Fourier transform infrared spectroscopy (FTIR) The structure and morphology of the Ni/MCM-41 were characterized by X-ray diffraction (XRD) and field emission transmission electron microscopy (FE-TEM) XRD results showed a well-ordered hexagonal pore structure, FE-TEM also revealed, as a complementary technique, the structure and pore size The textural properties of the Ni/MCM-41 were analyzed using N-2 adsorption isotherms at 77K The hydrogen-storage capacity of the Ni/MCM-41 was evaluated at 298 K/100 bar It was found that the presence of Ni on mesoporous MCM-41 created hydrogen-favorable sites that enhanced the hydrogen-storage capacity by a spillover effect Furthermore, it was concluded that the hydrogen-storage capacity was greatly influenced by the amount of nickel oxide, resulting in a chemical reaction between Ni/MCM-41 and hydrogen molecules. Crown Copyright (C) 2010 Published by Elsevier Inc All rights reserved.