It is essential to keep the balance among rolling resistance, wet skid resistance and wear resistance (the so-called devil's triangle) of tire treads so as to ensure the reliability and safety of the vehicles. For this purpose, hexamethyl-disiloxane (HMDS) and carboxylated polyethylene vinyl acetate copolymer (EVA, emulsion polymer latex) were used to modify nanosilica by in situ surface-modification method, thereby obtaining surface-capped nanosilica possessing good compatibility and strong interfacial interactions with rubber matrix. The surface-capped nanosilica of the above both modifications were introduced into the blend of solution polymerized styrene butadiene rubber (SSBR) and butadiene rubber (BR), and its effect on the mechanical properties and wear resistance of the SSBR/BR-matrix nanocomposites was investigated. The results indicated that both HMDS and EVA contribute to enhancing the compatibility and interfacial interactions of nanosilica with the rubber matrix, which is favorable for improving the mechanical properties and wear resistance of SSBR/BR-matrix nanocomposites. Particularly, HMDS can endow the rubber-matrix nanocomposites with increased wet skid resistance, and EVA can ensure the low rolling resistance of the nanocomposites. Therefore, the SSBR/BR blend filled with HMDS–SiO2–EVA possesses the desired mechanical properties and wear resistance and shows promising prospective as a candidate material for fabricating high-performance tire tread.