Mixtures of layered silicates (vermiculite and kaolinite) and carbon fibers were investigated as filler materials for polytetrafluoroethylene. The supramolecular structure and the tribological and mechanical properties of the resulting polymer composite materials were evaluated. The yield strength and compressive strength of the polymer increased by 55% and 60%, respectively, when a mixed filler was used, which was attributed to supramolecular reinforcement of the composites. In addition, the wear resistance increased by 850 times when using vermiculite/kaolinite fillers, which was due to protection of the surface by the formation of hard tribofilms.