Thiuram disulfides form synergistic combinations with thiazole and thiazole-based accelerators, namely, N-cyclohexyl-2-benzothiazole sulfenamide (CBS), 2-mercaptobenzothiazole (MBT), and 2-mercaptobenzothiazyl disulfide (MBTS). Unfortunately, widely used thiuram disulfides (TD) generate carcinogenic N-nitrosoamine. It is reported that the nitrosamines from N-methylpiperazine and dibenzylamine are free from this menace. So, some investigations were carried out with the binary combinations of each of bis(N-methylpiperazino)thiuram disulfide (MPTD), tetrabenzylthiuram disulfide (TBzTD), and tetramethylthiuram disulfide (TMTD) separately with CBS, MET, and MBTS. It was observed that all the TD are activated by the CBS, MET, or MBTS in the combinations studied. The intensity of activation is manifested in the enhancement of torque, modulus, tensile strength, cure rate, hardness, and decrease of elongation at break values and is very much dependent upon the ratio of the accelerators used. Considering the torque, modulus, tensile strength, and the elongation at break values, it appears that MPTD and TBzTD are capable of competing with the hitherto unbeaten TMTD as suitable accelerators for the vulcanization of rubber. Some investigations in respect to heat- and age-resistance behavior have also been carried out and the observed differences in the activities of various binary combinations have been explained through a mechanism. The results obtained with filled vulcanizates indicate that the binary systems comprising TD and MBTS provide fruitful results of which the TBzTD-MBTS combination seems to give the best cure and physical data for practical vulcanizates.