Abstract Polyurethane elastomer materials composited by milled fiberglass were prepared using toluene diisocynate, polyether, and butanediol. Infrared spectrum, wide angle X-ray scattering, thermogravimetric analysis, and SEM analysis were employed to characterize the developed composite materials in detail. Furthermore, various mechanical properties and wear behavior of the materials were investigated using universal materials testing machines and a wear tester. The results showed that the microstrucutres and properties of the composite materials could not be improved considerably until the content of fiberglass reached a critical level such as 5%. Once the content was larger than 15%, various mechanical properties, in particular, the strength and toughness could be significantly increased. Accordingly, the wear performance such as abrasion resistance was also improved. In addition, it was also found that the mechanical properties of the composites treated by the coupling agent are apparently better than those untreated by the coupling agent. Further analysis on the strengthening mechanism of the composites indicated that such improved mechanical properties were attributed to that the coupling agent could form a layer of fine and compact films on the surface of fiberglass, and therefore reinforce the connection between the milled fiberglass and substrates.