One of the most dramatic reductions in the wear of PTFE has been achieved by compositing PTFE with as little as 1–5 wt% of alumina particles; this has been reported to produce wear rates K ∼10−7 mm3/Nm. The mechanisms associated with this reduction in wear are multifaceted, including 1) preventing crack propagation and delamination of the PTFE wear surface, 2) promoting tribochemistry and more recently 3) tribologically-induced breaking of the filler into nanoscale fragments to stabilize and reinforce tribofilms. However, in an effort to keep experiments comparable, many of the studies throughout the literature have focused on a narrow contact pressure range. In these experiments, we explored the effects of contact pressure on the tribological behavior of different PTFE and alumina composites, one of which is reported to achieve ultra-low wear (∼10−7 mm3/Nm) and another that is reported to only have mild reductions in wear (∼1 × 10−5 mm3/Nm) compared to unfilled PTFE (∼4 × 10−4 mm3/Nm). We found that with decreased contact pressures, the PTFE-alumina composite that was previously reported as high wear could achieve ultralow wear rates. The PTFE-alumina composite previously reported to achieve ultralow wear achieved ultralow wear at a range of low to high contact pressures, with a higher pressure limit corresponding to increases in wear. The friction behavior of PTFE-alumina composites was found to be highly dependent on contact pressure, with increasing pressures resulting in decreasing friction coefficients (∼0.5–0.17 over a 0.62–8.5 MPa range). This effect became more pronounced when the contact pressure was incrementally varied during testing resulting in up to a 70% decrease or increase in friction coefficient due to increasing or decreasing the pressure, respectively. IR spectra of the polymer wear surface showed that tribofilms rich in carboxylates and metal oxides form at the full range of contact pressures tested, even at the extremes. This formation of tribofilms at the sliding interface not only contributes to the ultralow wear of these materials, but plays a role in the friction behavior observed. From this, we gained new insight into the role, functionality and limitations of the alumina fillers.