The influence of the novel vulcanizing agent, silica supported sulfur monochloride (silica-s-S), comparing with sulfur on the filler-rubber interfacial interaction, mechanical properties and the strain-induced crystallization behaviors were investigated. Due to the formation of interparticle domain, silica-s-S immobilized more rubber chains approaching its surface as the crosslinking points than sulfur vulcanization system. Furthermore, the tightly immobilized rubber chains on silica-s-S surface bring to the significant enhancement of mechanical properties of NR nanocomposites. Meanwhile, the immobilized rubber chains also induced the formation of highest initial crystallinity index and slower decreasing lateral crystallite size with increasing strain ratio. Silica-s-S with more tightly immobilized rubber chains approaching its surface shown better reinforcing effect and strain-induced crystallization behaviors on rubber than that of sulfur vulcanization system. (C) 2018 Published by Elsevier Ltd.