ABSTRACT High‐damping rubber materials are essential for fabricating high‐performance green tires due to their distinct advantage of low noise and vibration, good auto‐braking, and service life. However, the poor interfacial compatibility between the common nonpolar tread rubber materials and polar polymers/fillers severely restricts the development of high‐damping rubber composites. Herein, we prepared a multi‐functionalization high vinyl polybutadiene rubber (MFHVBR) without gel formation by anionic reaction. This significantly enhanced the interaction and compatibility with the high‐damping ethylene‐vinyl acetate (EVA) rubber. The interfacial potential energy of the MFHVBR/EVA blended system is nearly five times lower than that of the high vinyl polybutadiene rubber (HVBR) and EVA blended system, as certified by the molecular dynamics (MD) simulations. At an optimized MFHVBR/EVA weight ratio of 8:2, the composites demonstrate significantly improved damping performance without sacrificing the vulcanization rates and mechanical properties. The effective damping temperature range (tanδ > 0.3) from −11.1°C to 56.7°C totally covered the service temperature of tires and is also among the highest values for the reported tread rubber materials. The interfacial potential energy used for predicting the interfacial compatibility between the nonpolar rubbers and polar polymers/fillers provides insights for realizing high‐damping rubber composites.