Catalytic synthesis of multi-walled carbon nanotubes (MWNTs) by the pyrolysis of acetylene over mischmetal (Mm) based MmNi2 and MmFe 2 hydride catalysts is reported. The hydrogen decrepitation technique has been used to prepare the catalyst particles of these Mm based hydrogen storage alloys. Large hydrogen decrepitation and low cost make these hydrides potential catalysts for large-scale production of CNTs. The samples were purified by air oxidation and acid treatment and were characterized by XRD, SEM, TEM, HRTEM, Raman spectroscopy and XPS. The yield of MWNTs was estimated to be ∼60% and the purity of MWNTs thus obtained was more than 90%, as characterized by TGA. In addition, hydrogen adsorption measurements were carried out for as-prepared and purified MWNTs at 125 and 298 K using a high pressure hydrogen adsorption set-up. A maximum hydrogen storage capacity of 3.2 wt% at 60 bar is obtained at 125 K for purified CNTs prepared with MmFe2 hydride catalysts. © 2005 IOP Publishing Ltd.