An urchin-structured multiwall carbon nanotubes-hard carbon spherule (MWNTs/HCS) composite synthesized through acetylene pyrolysis is introduced in this article. In the composite, HCS is thoroughly coated by intercrossed MWNTs. Outstanding lithium uptake/release property is shown by this composite. Reversible charge capacity of 445 mAh g(-1) can be delivered by this composite after 40 cycles. It is found that the dramatic improvement may be attributed to the changes of Li-storage micropores and hydrogen element by introducing a MWNT coating. In addition, benefiting from the urchin structure and special preparation, the composite can deliver a reversible capacity of 245 mAh g(-1), even if the charge/discharge rate is 7 C. (C) 2008 The Electrochemical Society. [DOI: 10.1149/1.2980339] All rights reserved.