Supramolecular‐Reinforced Multifunctional Integrated Adaptive Coatings for Marine Protection

ABSTRACT Marine protective coatings often fail prematurely under the coupled effects of mechanical damage, UV irradiation, microbial fouling, and corrosion, because conventional barrier‑type systems lack adaptive interfacial regulation and integrated protective functions. Herein, a GO‑HHU‑CuPN‑EP coating is fabricated via a room‑temperature aqueous supramolecular self‑assembly strategy. In this coating, cerium‐based MOF nanocrystals (HHU) are grown in situ on GO nanosheets, followed by the surface assembly of a copper–tannic acid metal‐phenolic network (CuPN). The resulting hierarchical structure suppresses GO restacking and forms a tortuous diffusion barrier, while the CuPN acts as an interfacial regulator that improves filler‐matrix compatibility and environmental adaptability. The regulated interface enables efficient stress transfer, controlled inhibitor release, and photothermal defect confinement, while also improving weather resistance and antibacterial activity. As a result, the coating achieves a tensile strength of 27.4 MPa, an adhesion force of 7.4 MPa, an antibacterial rate of 96.2%, and an impedance modulus above 10 9.5 Ω·cm 2 after 100 d of immersion. These results establish supramolecular interfacial regulation as a coordinated strategy for integrating structural reinforcement and adaptive protection in durable marine coatings.