Aluminum is an attractive anode material for lithium ion batteries due to its low cost, high capacity and low equilibrium potential for lithiation/delithiation. The compact surface oxide layer is usually considered to be detrimental for lithium storage in Al due to its poor conductivity for Li+. Here we show that the Al oxide layer, which is positively charged, can be utilized to assist the homogeneous loading of the Al nanoparticles on to the negatively charged graphene oxide (GO) sheets. During the thermal reduction of GO to reduced GO (rGO), anhydrous HCl is introduced to selectively remove the surface oxide on the Al particles. The vitalized Al/rGO composite exhibits high lithium storage capacity of 1041mAhg−1 after 500 cycles at current density of 500mAg−1. The results demonstrate how the double edged surface oxide layer on Al nanoparticles can be manipulated to enable high performance lithium storage in Al, which is illuminating for the application of Al as a high performance, low cost anode material for lithium ion batteries.