A nanohybrid filler of functionalized graphene created with eco-friendly coupling agents (ECAs) and silica was fabricated by decorating silica onto graphene through a sol-gel process. To do this, relatively large high-quality graphene flakes with an extremely low oxygen content were fabricated using a ternary graphite intercalation compound method. The ECAs with hydrophobic and the hydrophilic groups mitigate graphene aggregation while also acting as an interfacial or bridging material. Furthermore, graphene-silica nanohybrids (GSNs) were incorporated by compounding to solution-styrene-butadiene rubber (SSBR) through mechanical mixing. The GSN-embedded SSBR matrix shows remarkable enhancements in the mechanical properties, thermal and electrical conductivities, and the gas barrier properties, even at a low loading rate, due to the efficient dispersion of GSNs, which enhances the interaction with the rubber matrix. The incorporation of GSNs improved the storage modulus considerably upon evolution of the filler network and with the creation of a crosslinking network of the composites