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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. 

Abstract Peptides naturally have stimuli‐adaptive structural conformations that are advantageous for endowing synthetic materials with dynamic functionalities. Here, we report a carbodiimide‐based approach, combined with electrostatic modulation, to instruct π‐conjugated peptides to self‐assemble and be responsive to thermal disassembly cues upon consumption of the assembly trigger. Quaterthiophene‐functionalized peptides are utilized as a model system herein to study the formation of nanostructures at non‐equilibrium states. Peptides were designed to have aspartic acid at the termini to allow intramolecular anhydride formation upon adding carbodiimide, which consequentially reduces the electrostatic repulsion and facilitates assembly. We show that the carbodiimide‐fueled assembly and subsequent thermally assisted disassembly can be modulated by the net charge of the peptidic monomers, suggesting an assembly mechanism that can be encoded by sequence design. This carbodiimide‐based approach for the assembly of designer π‐conjugated systems offers a unique opportunity to develop bioelectronic supramolecular materials with controllable formation of dynamic and stimuli‐responsive structures.