A facile and low-cost electroless deposition technique is utilized to decorate multi-walled carbon nanotubes (CNTs) with Ni. The obtained composites are attempted to use as hydrogen storage materials, whose performance is evaluated with a high-pressure microbalance. Effects of the concentration of plating solution, deposition time, and reaction temperature on the loading amount, particle size, morphology, and distribution density of Ni are studied using a transmission electron microscope. With proper deposition parameters, highly dispersed Ni nanoparticles with a uniform diameter can be fabricated on CNTs, causing a notable hydrogen spillover reaction on the composite. The optimum hydrogen storage capacity of the prepared Ni-decorated CNTs with a average diameter of 5 nm, measured at 6.89 MPa and 25 degrees C, is 1.02 wt%, which is almost three times higher than that (0.35 wt%) of pristine CNTs. (C) 2010 Professor T. Nejat Veziroglu. Published by Elsevier Ltd. All rights reserved.