 Aluminum–nickel/multiwall carbon nanotubes (Al–Ni/MWCNTs) composites have been prepared and tested as a new type of anode material. First, core–shell aluminum–nickel composite particles were fabricated using an electroless deposition of nickel onto the aluminum. Then, Al–Ni/MWCNTs composites were prepared by combining different amounts of MWCNTs (10, 20, 40 wt%) using a planetary ball milling method. The morphologies and structures of the produced Al–Ni/MWCNTs composite powders were characterized using scanning electron microscopy, and energy dispersive spectroscopy was used to understand the elemental surface composition of composites. X-ray diffraction analysis was performed to investigate the structure of the Al–Ni/MWCNTs composite powders. To investigate the electrochemical performance of Al–Ni/MWCNTs composite electrodes, charge/discharge tests and cyclic voltammetry were performed using the produced cells. The amount of MWCNTs was shown to be critical to improving the Al–Ni/MWCNTs composite anodes with respect to cyclability and stability.