Robust Chiral Metal–Organic Framework Coatings for Self‐Activating and Sustainable Biofouling Mitigation

Abstract Surface coatings are designed to mitigate pervasive biofouling herald, a new era of surface protection in complex biological environments. However, existing strategies are plagued by persistent and recurrent biofilm attachment, despite the use of bactericidal agents. Herein, a chiral metal–organic framework (MOF)‐based coating with conformal microstructures to enable a new anti‐biofouling mode that involves spontaneous biofilm disassembly followed by bacterial eradication is developed. A facile and universal metal‐polyphenol network (MPN) is designed to robustly anchor the MOF nanoarmor of biocidal Cu ²⁺ ions and anti‐biofilm d ‐amino acid ligands to a variety of substrates across different material categories and surface topologies. Incorporating a diverse array of chiral amino acids endows the resultant coatings with widespread signals for biofilm dispersal, facilitating copper‐catalyzed chemodynamic reactions and inherent mechano‐bactericidal activities. This synergistic mechanism yields unprecedented anti‐biofouling efficacy elucidated by RNA‐sequencing transcriptomics analysis, enhancing broad‐spectrum antibacterial activities, preventing biofilm formation, and destroying mature biofilms. Additionally, the chelation‐directed amorphous/crystalline coatings can activate photoluminescent properties to inhibit the settlement of microalgae biofilms. This study provides a distinctive perspective on chirality‐enhanced antimicrobial behaviors and pioneers a rational pathway toward developing next‐generation anti‐biofouling coatings for diverse applications.