A composite of Ti-V-based bcc phase alloy surface-modified by multiwalled carbon nanotubes (MWNTs) was prepared simply by a short-time ballmilling process. The composite sample showed remarkably improved electrochemical hydrogen release capacities. For the 30 min ballmilled Ti-30V-15Mn-15Cr + 10 wt % MWNTs sample, a discharge capacity of 1200 mAh g(-1) was obtained at a discharge current of 10 mA g(-1) and 353 K. The high capacity was due to a synergetic action of the two materials, which not only induced the Ti-30V-15Mn-15Cr alloy to release hydrogen more easily but also increased the hydrogen storage in the carbon component. (c) 2005 The Electrochemical Society.