τ likewise increases with Σ, but then levels off above a critical value. These results are explained by the molecular friction of the adsorbed polymer chains sliding along the rubbery polymer matrix. The results can be used to guide the interfacial design of polymer nanocomposites to obtain ultimate macroscopic mechanical control. In particular, the monomeric friction coefficient, ξ 1 , could be used to adjust the macroscopic properties of this type of nanocomposite.