<p>The copper in friction composites poses adverse risks to both the environment and human health; its suitable alternatives have attracted great attention. Toward this aim, the Cu-free phenolic friction composites were designed and fabricated to study the friction-wear synergies of carbon fiber (CF) and aramid pulp (AK), as well as the favorable tribosurface. The process flow of each specimen was as follows: mixing and drying, hot-pressed molding, post-treatment and surface finishing. Moreover, all of the parameter setting remained unchanged. The friction-wear behaviors were tested at 100, 150, 200, 250, 300 and 350&#xa0;°C by a constant-speed friction tester. The surfaces were characterized and analyzed using an optical microscope, as well as SEM coupled with the element mappings. It is indicated that the friction-wear synergies of CF and AK, including positive and negative ones, are closely related to mass ratios of CF to AK and their sum mass percentages in the composites. The superior behaviors of independent friction and wear are the combinations of 1:4 of CF to AK with sum percentage of 1 wt.% and 2:3 with sum percentage of 3 wt.%, respectively. However, either 3:2 or 4:1, together with sum percentage of 5 wt.%, manifests negative synergies. The best friction specimen increases friction coefficient by above 27% at higher temperature compared the least friction one, and the best anti-wear specimen reduces the total mass ratio more 35% than ones containing single CF or AK in the same series. Besides, higher CF mass percentages worsen the friction-wear undulations. The tribofilms are heterogeneous on the counterface, and their continuity and compactness are beneficial for the friction-wear behaviors. The findings will assist in gaining an insight into friction-wear mechanism and developing high-quality friction composites.</p>