For rubber vulcanizates or crosslinked rubbers, inherent characteristics of rubber elasticity are well known to be mainly controlled by the change in conformational entropy under deformation, causing constrained molecular mobility of rubbery network chains. In this part II of special lecture, 1H-pulsed NMR method is applied to observe the motional heterogeneity in the crosslinked rubbers, related to effects of crosslink density and incorporation of reinforcing carbon black fillers on the tensile failure behaviors under various conditions. Furthermore, as for analysis of thermo-oxidative aging behaviors for the crosslinked rubbers, the relationships between the breaking stretch ratio in tensile measurements, É b, and NMR relaxation properties such as spin-spin relaxation time, T2, and residual dipolar coupling constant , Dres, were discussed to predict the failure properties of small pieces sampled from engineering rubber parts, for which tensile tests could not be easily performed.