This work investigates natural rubber (NR) composites vulcanized with different combinations of accelerators in efficient cure systems. The NR compounds were characterized for cross-link density, hardness, tensile strength, and dynamical–mechanical properties, before and after aging. Among the cure systems used, that containing the highest amount of free sulfur presented the best mechanical performance, before and after aging; concerning dynamic properties after the aging, the composition with a lower number of cross-links was the best.