This study explored the possibility of preparing a new thio accelerator, N-benzylimine aminothio-formamide to investigate its synergic accelerator activity in three conventional binary accelerator systems, N-cyclohexyl benzothiazyl sulfenamide, mercapto benzothiazyl disulfide, and tetramethylthiuram disulfide in the sulfur vulcanization of natural rubber. Each system was found effective in reduction of cure time as a further proof of the nucleophilic mechanism suggested in the earlier reports. The vulcanizates of the mixes of the three systems were experimented for evaluating their physicomechanical properties. Most of the properties were found better than those of the reference mixes. Crosslinks were also evaluated for correlating the properties. Based on the evaluated properties, optimum dosage of the new binary systems were derived. (C) 2010 Wiley Periodicals, Inc. J Appl Polym Sci 116: 2976-2981, 2010