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A mussel-inspired mechanism was used to solve the problem of filler aggregation in rubber composites. This research aims to improve carbon black (CB) dispersion in epoxidized natural rubber (ENR) composites through π−π stacking and cation−π interactions by adding dopamine (D). In this study, various aromatic interactions (π−π stacking and cation−π interactions) between the D-functionalized ENR molecules and the surface of the CB were observed by Fourier transform infrared (FTIR) and Raman spectroscopy. Notably, the small and wideangle X-ray scattering (SAXS/WAXS) analyses supported our inference from the rubber processing analysis (RPA) and transmission electron microscopy (TEM) results that the aromatic interactions enhanced the CB dispersion in ENR composites. This phenomenon improved the tensile strength (138%), Young’s modulus (93%), and energy-saving properties (50%). Finally, this research provided an alternative strategy using mussel-inspired material to solve the CB aggregation problem in rubber products, yielding ENR composites with superior performance properties.