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Although the size effects of a filler are closely related to the complex multi-level structures of their polymer com-posites;unfortunately, such relationships remain poorly understood. In this study, we investigated the effects of various sizes (40–600 nm) of silicon carbide (SiC) fillers on the wear behavior of ultrahigh molecular weight polyethylene (UHMWPE) in the presence of the silane coupling agent KH-560. All of these SiC fillers improved the wear resistance of UHMWPE significantly, with a medium size (150 nm) being optimal. To examine the rea-sons for this behavior, we analyzed the multi-level structures of the samples in terms of their matrix structures (crystalline;amorphous;interphase), matrix–filler interactions (physical adsorption;chemical crosslinking;hy-brid network) and the extal effects of SiC fillers (bearing loads;transferring frictional heat). The high rigidity and thermal conductivity of SiC fillers and, more importantly, the intrinsic characteristics of the matrix structures (larger crystal grains;higher interphase;stronger amorphous entangled networks) were the key parameters af-fecting the enhancement in the wear-resistance of the UHMWPE. Herein, we also provide interpretations of the corresponding physical effects. Our results should improve our understanding of the structure–property relation-ships and, thus, should guide the formula design of UHMWPE composites.