Constructing Self‐Renewing Silicone‐Hydrogel Hybrid Coatings with Integrated Fouling Resistant/Release/Killing Mode toward Superior Biofouling Defense

Abstract Silicone hydrogel coatings, which integrate fouling self‐release and fouling resistant properties, represent a groundbreaking advancement in environmentally friendly biofouling mitigation, but are still plagued by static fouling conditions and longevity concerns. In this work, Schiff base chemistry and a sol‐gel technique is leverage to develop degradable silicone‐hydrogel hybrid antifouling coatings by incorporating amphiphilic silicone‐based polymers with terephthalaldehyde (TPE) and cinnamaldehyde (CAL). The synergistic combination of flexible Si─O bonds in the polymer backbone and reversible covalent crosslinking imparts exceptional flexibility (hardness of 0.135), controlled degradability, and dynamic surface self‐renewal capabilities, ensuring sustained antifouling performance through surface dynamic stability. During degradation, the amphiphilic polymers will self‐enrich at the interface, forming a dual‐functional surface that combines fouling release and fouling resists properties. The antibacterial TPE and natural CAL, anchored within the polymer network, exhibit environment‐responsive release behavior, effectively suppressing bacterial proliferation and biofilm adhesion. The optimized coating achieves a bactericidal rate of 98.8%, an anti‐bacterial adhesion rate of 99.8%, and a predicted anti‐fouling longevity of 5.5 years with a thickness of 200 µm. This innovative approach enables a new anti‐biofouling coating that involves unique fouling control mode, thereby meeting the diverse application.