Carbon nanotubes (CNTs) are considered to be excellent candidates for high performance electrode materials in Li ion batteries. The nanometer-sized pore structures of CNTs can provide the hosting sites for storing large numbers of Li ions. A short diffusion distance for the Li ions may bring about a high discharge rate. The long-cycle performance of aligned multiwalled carbon nanotubes (MWNTs) directly synthesized on stainless-steel foil as an anode material in lithium battery is demonstrated. An increase in the specific capacity with an increase in the cycle number is observed. Starting at a value of 132 mA hg−1 in the first cycle at a current rate of 1 C, the specific capacity increased about 250% to a value of 460 mA hg−1 after 1 200 cycles. This is an unusual but a welcoming behavior for battery applications. It is found that the morphology of the MWNTs with structural and surface defects and the stainless-steel substrate play an important role in enhancing the capacity during the cycling process.