Graphene nanoparticles (GNPs) added styrene-butadiene-styrene (SBS)-modified asphalt suffers from serious compatibility and agglomeration problems. To tackle these problems, in this study, graphene oxide (GO) was mixed with bromobutane to synthesize butylated graphene oxide (C 4 H 9 -GO) composite, which was in turn compounded with SBS for the preparation of C 4 H 9 -GO/SBS-modified asphalt. C 4 H 9 -GO/SBS-1.0-modified asphalt exhibited the best performance in terms of 11.4% increased softening point, 19.3% increased ductility, and 10.2% reduction in penetration as compared to 5% SBS-modified asphalt. Dynamic shear rheometer and multistress creep recovery tests showed that at 1.0% C 4 H 9 -GO contents, C 4 H 9 -GO/SBS composite-modified asphalt exhibited the best high-temperature performance and low stress sensitivity. Microscopic characterization of C 4 H 9 -GO via Fourier transform infrared spectroscopy, X-ray diffraction, and Raman spectroscopy revealed successful bonding between C 4 H 9 and GO, increasing interlayer spacing in GO. Atomic force microscopy and scanning electron microscopy analysis showed the superior elasticity of C 4 H 9 -GO than GNPs. Differential scanning calorimetry analysis indicated that C 4 H 9 -GO sheets can be stabilized by SBS through π-π stacking with the polystyrene chains. This study awarded to the preparation of novel C 4 H 9 -GO/SBS-modified asphalt with superior mechanical property can be deemed of potential value and applications in construction and highway industries.GNPs have also been applied as modifiers for the preparation of modified asphalts. Han et al., 10 via in situ polymerization strategy, synthesized polystyrene-GNPs (PS-GNPs) and added them to styrene-butadiene-styrene (SBS)-modified asphalt, which exhibited improved softening point and high-temperature rutting resistance performance than the parent asphalt. The National Cooperative Highway Research Program found that compared to conventional asphalt binders, GNPs-enhanced asphalt binders exhibit excellent flexural strength at low temperatures, but the fracture energy of Additional Supporting Information may be found in the online version of this article.