This study investigates the impact of a binary filler on the physicomechanical and tribological properties, as well as structure, of polymeric composite materials based on ultra-high-molecular-weight polyethylene. The organic modifier—2-mercaptobenzothiazole and wollastonite particles synthesized from two different systems (modeled and derived from waste) were used as the binary filler. The synthesis of wollastonite was carried out in the complex model system (CaSO4·2H2O–SiO2·nH2O–KOH–H2O) and from technogenic waste (borogypsum). It was demonstrated that the introduction of the binary filler made it possible to obtain an optimal combination of mechanical and tribological properties. It was found that during the wear of polymeric composite materials loaded with organic fillers, the fillers migrate to the friction surface, providing a shield against abrasive wear of the steel counterface. Due to the modification of ultra-high-molecular-weight polyethylene by 2-mercaptobenzothiazole, the interdiffusion of polymeric matrix macromolecules and interphase coupling with wollastonite particles improve. The 2-mercaptobenzothiazole organic compound used as the filler facilitates the relaxation processes within the composite under external loads.