ABSTRACTHigh‐vinyl polybutadiene rubber (HVBR) and solution‐polymerized styrene–butadiene rubber (SSBR) can meet the requirements of high‐performance tires due to their excellent wet skid resistance and lower rolling resistance. In this paper, the effects of the vinyl and phenyl groups and their contents on the vulcanization behavior, mechanical strength, fatigue resistance, heat resistance, and wear resistance of HVBR and SSBR were investigated, and the dynamic viscoelasticities of HVBR and SSBR vulcanizates with or without carbon black were explored by dynamic mechanical analysis (DMA). The experimental results showed that the vinyl groups contributed more to the wear resistance and fatigue resistance of vulcanizates than the phenyl groups, but the phenyl groups contributed more to the mechanical strength of the vulcanizates than the vinyl groups. The DMA results showed that the vinyl and phenyl groups could significantly improve the road‐gripping capability and wet skid resistance of HVBR and SSBR vulcanizates, but carbon black could slightly weaken the effect of vinyl and phenyl groups on the wet skid resistance of vulcanizates, and the effect of carbon black on vinyl groups was more significant. Despite the presence of carbon black, the phenyl groups contributed more heat buildup to the vulcanizates than the vinyl groups. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 45975.