The assembly of nanostructured materials with tunable properties is of growing interest across fundamental research and industrial applications. Polyphenol-functionalized polymers, which integrate phenolic moieties within polymer backbones, have emerged as versatile building blocks for engineering nanostructured materials with controlled size, morphology, composition, and functionality. Owing to the chemistry of polyphenols, polyphenol-functionalized polymers enable diverse assembly pathways through covalent and noncovalent interactions with metal ions, small molecules, macromolecules, and nano/microstructures, allowing fine control over the physicochemical properties of the resulting materials. In this review, we provide a structured overview of polyphenol-functionalized polymers, beginning with key synthetic strategies, including ring-opening polymerization, radical polymerization, controlled/living radical polymerization, and post-modification of preformed polymers. We then discuss the assembly behaviors of these polymers, driven by synergistic interactions between the polyphenol groups and polymer chains, highlighting metal coordination, molecular complexation, and integration with nano/microstructures. These interactions result in assembled materials with tunable physicochemical properties, including surface charge, hydrophobicity–hydrophilicity balance, biocompatibility, stealth and targeting, stimuli-responsiveness, and bioactivity. Finally, we highlight emerging applications of polyphenol-functionalized polymers in multifunctional interfaces, responsive and adaptive materials, energy and electronic devices, and biomedicine. Overall, this review provides a concise and up-to-date overview of the synthesis, self-assembly mechanisms, and physicochemical tunability of polyphenol-functionalized polymers, and their wide application in materials engineering.
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