In the present work, uncured and cured properties of high-performance, sustainable Natural Rubber nanocomposites developed by leveraging the unique synergy between carbon black and fibrous nanofillers such as silicon carbide, carbon nanotubes, and aramid nanofibers were investigated. Reinforcement in these composites was analyzed using the properties of the unvulcanized compounds, which were then correlated with those of the vulcanized compounds. A 50% increment was recorded for the bound rubber content of the nanocomposites, which resulted in tremendous improvements in the reinforcement index and tensile strength of the unvulcanized nanocomposites. In contrast, the die swell index came down compared with the control compound. The formation of a percolating network due to the presence of high aspect ratio fibers resulted in a higher Payne effect in hybrid nanocomposites, which was confirmed from the scanning and transmission electron microscopy. The 100% modulus, 300% modulus, and tensile strength of the unvulcanized nanocomposites recorded an improvement of 80, 121, and 450%, respectively, by the incorporation of nanofibers. The molecular aspects of reinforcement were elucidated from theoretical calculations using Mooney-Rivlin plots. It was presumed that the improved reinforcing efficiency of the nanofibers resulted from restricted mobility of elastomer chains due to the presence of the dual filler system.