It is well known that surface of ZnO acts both as a reactant and a catalytic reaction template in rubber vulcanization by activating and bringing together reactants. The particles of accelerators, fatty acid, and sulfur diffuse through the polymer matrix and get adsorbed on the surface of ZnO, forming intermediate complexes.Hence dispersion of ZnO in the elastomer matrix is a determining parameter. Capping is one of the novel techniques for increasing ZnO-stearic acid/accelerator interaction, thereby enhancing their activities. During the sol-gel precipitation of nano ZnO, if a suitable capping agent is added, agglomeration of ZnO particles gets reduced, leading to the formation of nano particles. Since only very few studies are found reported on synthesis of acceleratorcapped ZnO and its application in rubber vulcanization, attempts have been made in this study to synthesize our novel accelerator N-benzylimine aminothioformamide (BIAT)-capped-stearic acid-coated nano ZnO (ZOBS), and BIAT-capped ZnO (ZOB) to investigate their effects in natural rubber (NR) vulcanization. Efforts have also been made to synthesize stearic acid-coated nano zinc phosphate (ZPS) with an aim to find an alternative to conventional ZnO in vulcanization. Mechanical properties like tensile strength, tear resistance, abrasion resistance, and compression set were found out. Swelling values of the vulcanizates as a measure of crosslink densities were also determined. Optimum dosage of ZOBS and a combination of ZOB and ZPS were also derived and found that capped ZnO is superior in NR vulcanization to conventional ZnO in improving cure properties including scorch safety and mechanical properties.