A simple and efficient devulcanization process assisted by a proprietary devulcanizing agent (DVA) is presented in this paper. The effect of concentration of DVA (0-6 phr) and the effect of cure system i.e. CV, semi-EV and EV systems used for vulcanization of original sample on the efficiency of devulcanization of carbon black filled natural rubber (NR) vulcanizates was studied. The efficiency of devulcanization and the crosslink distribution pattern of the original as well as the devulcanized samples were estimated by determining the residual crosslink density and chemical probe analysis respectively. Maximum retention of tensile and tear strengths was accomplished by semi EV samples where as maximum processability and devulcanization percentage were associated with EV samples. The chemical probe analysis of the devulcanized sample showed that mechanical shearing predominantly breaks the majority crosslink type. Finally, a commercial devulcanized rubber was reworked with phr DVA and the residual crosslink density reduction accomplished with a resultant improvement in mechanical properties further ascertained the role of DVA as a devulcanizing aid.