ABSTRACT This study explores the use of carbon nanotube (CNT) clathrates with internally loaded lubricant additives—as a reinforcing phase to prepare polymer composites, which can enhance both the lubrication characteristics and mechanical strength of the resulting composites. Two types of CNT clathrates were first synthesized and then used to reinforce three different polymer matrices, and the effects of filling content on the mechanical and tribological properties were investigated, along with the influence of test load and speed. The release and self‐lubrication mechanism of the CNT clathrates within the composites during friction were also explored. Results indicated that incorporating CNT clathrates improved the tensile strength by about 45% with an optimal filler content around 5 wt.%, and the friction coefficient and the wear rates could be reduced by 22% and 25%, respectively, compared with those of polymer matrices under this content. As testing speed and load increased, CNT clathrates further reduced the friction, though wear rates increased. During friction, the CNT clathrates released internal additives to form a self‐lubricating layer, thereby contributing to reduced friction and enhanced wear resistance.