Thermoplastic elastomers (TPEs) and metallic glasses (MGs), both lack of long-range ordering structure, have different physical and mechanical properties. To combine unique viscoelasticity of elastomers and excellent wear resistance of MGs, we propose to introduce a Pd40Ni40Si4P16 MG into a commercial styrene-butadiene-styrene (SBS) TPE to form MG/TPE composites. Serving as a hard and strong second phase dispersed in the SBS matrix, the micrometer-sized MG particles can effectively improve the wear resistance of the matrix due to a strengthening effect. In particular, the MG/TPE composite with an addition of 60 wt% MG shows significantly enhanced wear resistance up to about three times that of the SBS matrix. The present results provide a new way to enhance the wear resistance of the widely used TPEs, which may generate immense economic value by extending their service life.