With the emerging concerns on the use of nitrosamine evolving accelerators, safer alternatives are desirable for the rubber industry. In the present study, cure characteristics, physicomechanical properties, crosslink density, aging, dynamic mechanical, and thermal properties of vulcanizates prepared with two nitrosamine safe binary accelerator systems containing diisopropyl xanthogen polysulfide (DIXP) and tetrabenzyl thiuram disulfide (TBzTD), and DIXP and dibenzyl dithiocarbamate (ZBeC) were investigated for efficient sulfur vulcanization of natural rubber (NR) compounds. Synergistic effect in both cure and physicomechanical properties was observed for all the combinations of the two accelerator systems. The composition containing DIXP with a lower loading (0.6 phr) of TBzTD, and ZBeC, demonstrated the highest technological performance. Retention of tensile properties on oxidative aging was highest for the vulcanizate prepared with DIXP/TBzTD (1.4/0.6). Dynamic mechanical and thermogravimetric analysis further confirmed the crosslink density and thermal stability of the network structure of the binary systems. In overall, DIXP shows the potential to be used as a safer accelerator in the manufacture of appropriate dry NR-based rubber products.