To adapt to the complex application of polyurethane bearings, it is feasible to improve the tribological performance of single polyurethane-based friction materials through the synergistic effect produced by multi-component-lubricating fillers. In this context, rather than using tungsten disulfide (WS2), which has demonstrated excellent self-lubricating performance as a lubricating oil additive, this paper proposes that WS2 and single-walled carbon nanotubes (SWNTs) can be designed for addition into a polyether 4,4'-diphenylmethane diisocyanate (MDI) polyurethane matrix as self-lubricating fillers so as to explore the synergistic effect of micro- and nano-lubricating fillers on the tribological performance of polyurethane matrix materials. Through a series of characterizations and tests, it was found that the dispersion of two-component-lubricating additives in a polyurethane matrix is improved when the ratio of WS2 to SWNTs is roughly 2:1. In this case, the tribological performance of polyurethane matrix composites is more satisfactory than at other ratios. In addition, compared with the blank sample, the tribological performance of the synergistically modified polyurethane composites under dry friction is more significantly improved with the increase in contact load, while there is no significant improvement under water lubrication. Aside from contributing to the idea of exploring the synergistic effect of WS2 and other micro or nanofillers, this method also opens up the possibility of practically applying WS2 in the field of friction.