Interfacial modular assemblies of versatile polyphenols have attracted widespread interest in surface and materials engineering. In this study, natural polyphenol (tannic acid, TA) and nobiletin (NOB) can directly form binary carrier-free spherical nanoparticles (NT NPs) through synergistically driven by a variety of interactions (such as hydrogen bonding, oxidative reactions, etc.). The synthesis involves polyphenolic deposition on hydrophobic NOB nanoaggregates, followed by