An aromatic copolyester liquid crystal polymer (LCP) was introduced into carbon-fiber-reinforced polyamide–polyurethane (CF/PA-PU) composites through melt blending to improve the tribological properties of the composites. The effects of LCP on the mechanical, processing, and thermal properties of CF/PA-PU composites were compared to those of commonly-used graphite (Gr). The results showed that at 5 wt.% LCP content, the coefficient of friction (COF) was decreased by 16.06%, and the wear rate by 32.22% in the LCP/CF/PA-PU composite compared to the CF/PA-PU composite. Furthermore, using LCP instead of Gr showed significantly improved mechanical properties and reduced processing viscosity. The tensile strength of 5%LCP/CF/PA-PU composite could reach 99.08 MPa, while the equilibrium torque was reduced, being 26.85% higher and 18.37% lower than those of CF/PA-PU composite, respectively. The thermal stability of LCP/CF/PA-PU composites was also enhanced. The addition of 5 wt.% LCP to CF/PA-PU composite increased the initial decomposition temperature by 14.19% compared to CF/PA-PU. In sharp contrast, the addition of Gr increased equilibrium torque and actual processing temperature leading to processing difficulties and instability. This approach offers a novel strategy for tribological applications and tackles the problem of high viscosity in CF/PA-PU composites.