Durable Adhesion in Polyphenol Hydrogel Adhesives: From Interface Aging to Long-Term Stabilization

Polyphenol hydrogel adhesives have found broad application in wound management, tissue repair, leak sealing, and biointegrated systems due to their robust wet adhesion, versatile interfacial reactivity, and broad substrate adaptability. However, they often suffer from progressive interfacial aging, leading to diminished interfacial retention, compromised sealing integrity, and reduced functional stability during service. Improving interfacial retention is therefore critical for extending their utility in biomedical environments. This review begins by examining the time-dependent evolution of polyphenol hydrogel adhesive interfaces, highlighting the major mechanisms underlying adhesion degradation and the corresponding stabilization principles. We further summarize emerging strategies for long-term interfacial stabilization and outline future directions in interface-specific material design and performance assessment. By providing a comprehensive framework for understanding durable polyphenol-mediated adhesion, this review aims to guide the rational development of next-generation bioadhesives for increasingly demanding biomedical applications. STATEMENT OF SIGNIFICANCE: Polyphenol hydrogels have emerged as versatile wet adhesives for tissue sealing, wound protection, drug delivery, and dental treatment. Recent studies increasingly focus on whether these materials can maintain adhesion under physiological conditions over time. This Review discusses the time-dependent evolution of polyphenol-mediated interfaces, major causes of adhesion loss, and current strategies for improving interfacial retension. Future work should place greater emphasis on long-term testing under realistic service conditions, comprehensive biosafety assessment, and clinical translation. By integrating these aspects, this Review aims to support more reliable evaluation and guide the development of durable polyphenol hydrogel adhesives for wet, dynamic, and demanding biological environments, with improved safety, reliability, and translational potential.