The present study aims to find the correlation between the crosslink density of the freshly prepared sample tobe devulcanised and the efficiency of mechanical devulcanization in a two roll mill. Efficiently vulcanized(EV) carbon black filled natural rubber vulcanizates with varying crosslink densities were mechanicallydevulcanised on a two-roll mixing mill and the efficiency of devulcanization was determined from the residualcrosslink densities of the devulcanized samples and the corresponding revulcanizate properties. With increasingcrosslink density of the starting material, the tear and tensile strengths of the sample first increased, reached amaximum and then decreased. The percent devulcanization associated with these samples on mechanicaldevulcanization ranged between 70-80 per cent irrespective of their difference in original crosslink density.Hence, the absolute value of the residual crosslink density is high when the original crosslink density is highleading to poor revulcanizate properties irrespective of the higher per cent devulcanization attained. Thus, theoriginal crosslink density of the sample to be devulcanized appears to be one of the most important factors thatdefines the revulcanizate properties of the devulcanized samples.