Hybrid nanocomposites were prepared by predispersion of new nanofibers such as aramid nanofibers, carbon nanotubes, silicon carbide nanofibers (SiC), cellulose nanofibers, and graphite nanofibers in natural rubber (NR) latex prior to melt mixing in an internal mixer to ensure the exquisite dispersion of nanofibers in NR. The competency of these nanofibers in reinforcing NR as well as enhancing its barrier properties has not been widely investigated. The fabricated nanocomposites showed enhanced curing as well as mechanical and dynamic mechanical properties. Morphology of the composites was analyzed through electron microscopy. The increase in tortuosity created by the presence of the hybrid filler system consisting of carbon black and nanofibers was studied using permeability models. At higher tearing energies, it was seen that the nanofiber-reinforced composites showed comparable crack growth properties; however, at lower energies, the fabricated composites exhibited higher crack propagation rates compared with the control compound when studied using a tear fatigue analyzer. The improved mechanical, dynamic mechanical, and barrier properties along with comparable fatigue crack growth properties offer an opportunity to apply these systems in high-end applications such as a thinner tire inner liner with a higher NR blend ratio, which can result in improved processability and reduced hysteresis, fuel consumption, and cost.