Modulating the Interactions of Peptide‐Polyphenol for Supramolecular Assembly Coatings with Controllable Kinetics and Multifunctionalities

Polyphenols and peptides represent two fundamental building blocks in the kingdom of supramolecular assembly (SA) coatings, which have recently attracted considerable interest. Regulating the assembly kinetics of SA coatings is critical to controlling the performance of SA coatings, but this area is still in its infancy, especially in the SA coating of peptide-polyphenol. Herein, a library of oligopeptides with rich diversity, numerous polyphenols, and modulators are explored to reveal their roles in the formation and regulation of SA coating. Citric acid (CA) is an effective regulator of interaction between the polyphenols and peptides to produce peptide-polyphenol coatings, TCP. The electrostatic interaction between tannic acid (TA) and cationic peptide drives the formation of TCP, while the multiple hydrogen bonds between CA and TA and peptide dominate the assembly kinetics. With optimized assembly pH and the mass ratio of TA, CA, and peptide, the thickness of TCP coating deposits onto diverse substrates (glass, silica, titanium, polystyrene) is ≈400 nm with controllable kinetics. The multifunctional TCP coatings are endowed via peptide-coupled functional units, including enhanced cellular adhesion, elevated osteogenic capacity, anti-protein adsorption, and antimicrobial. This work contributes to the understanding of the assembly kinetics and functionalization of peptide-polyphenol coatings.