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Natural rubber (NR) and functionalized graphene sheets (FGSs) nanocomposites were prepared by conventional two-roll mill mixing. The morphology and structure of the FGS was characterized confirming the successful exfoliation of the FGS. The strong rubber-to-filler interactions accelerate the cross-linking reaction, increase the electrical conductivity and cause an important enhancement on the mechanical behavior of the NR nanocomposites. The nanofiller does not affect the molecular dynamics of NR, while the presence of vulcanizing additives slowdowns the segmental motions and decreases slightly the time scale of the global chain dynamics in NR/FGS nanocomposites. These functional properties make NR/FGS nanocomposites a promising new class of advanced materials.