The tribological properties of aligned CNT/fullerene-epoxy nanocomposites were studied by nanoscratch, nanowear, and nano-indentation tests. Compared with neat epoxy, aligned CNT/fullerene-epoxy nanocomposites showed lower friction coefficient in scratch tests, a reduction of 38.1 and 26.2%, respectively. In addition, the aligned CNT-epoxy composite showed better wear resistance and its hardness and Young's modulus increased by 29.4 and 16.8%, respectively. In contrast, for a fullerene-epoxy nanocomposite with 10 wt% fullerenes, the hardness decreased by 50% and the Young's modulus decreased by more than 60% when compared with the neat epoxy.