Silica has recently attracted attention as reinforcing filler for tread formulations leading to lower rolling resistance and hysteretic losses with the development of “green tires” in the tire industry. Due to the poor compatibility of hydrophilic silica with a hydrophobic rubber, zinc-free coupling agents (ZFCs) are required to satisfy environmental concerns. In this work, we synthesized ZFCs and ZFCs-functionalized graphene (GZFCs), and fabricated GZFCs-embedded SBR with remarkable enhancement in mechanical, thermal, and electrical properties. The GZFCs-rubber composite showed enhanced dry and wet braking and rolling resistance due to enhanced dispersion and strong interfacial interaction of GZFCs in the silica/rubber matrix.