To improve interaction on the phase boundary of polymer composites, we used functional additives, mechanoactivation method, and ultrasound. In the case of the use of serpentine as a modifier of polytetrafluoroethylene (PTFE), the introduction of magnesium nanospinel (NS) as functional additive resulted in the increase of wear resistance of composite in 2500 times. Effect of ultrasonic irradiation on the composites comprising phlogopite was considered. IR data have shown that NS influences the intensification of the tribological processes. In sonicated composites the intensity of the IR spectra of oxidized fragments depends on the content of NS and correlates with the wear resistance.