This study explores the potential application of waste rubber (WR) as sustainable recycled rubber aggregates (RRA) in the construction sector. A layer of graphene oxide (GO) was coated on RRA through multiple surface modification techniques, aiming to enhance the interfacial properties in RRA mortars. The C-S-H phases were first tailored through chemical synthesis to better understand the nucleation and growth of hydration products with the presence of GO. Subsequently, a 180 ± 10 nm-thick GO coating was attached to the RRA surface through surface treatment with sodium hydroxide solution, silane coupling agent, and GO suspension. In addition, the mechanical strength, damping performance, water absorption, chloride resistance, and microstructural properties of cement mortars prepared with RRA were further assessed. It was found that the GO coating significantly improves the bonding between RRA and the cementitious matrix due to its hydrophilicity and nucleation effects, which locally facilitate the cement hydration at interfaces. The cement mortars produced with surface-modified RRA exhibit promising high-damping characteristics, accompanied by improved durability and mechanical performance over those prepared with untreated RRA.