This study reports a facile approach to construct versatile zein-polydopamine-casein coreshell nanocomposites (ZPCs) for polyphenol delivery systems. The surface of zein particles was first modified with mussel-inspired polydopamine (PDA), and then coated with casein, forming stable colloidal particles against environmental stresses including pH, salinity, storage, redispersion, and UV irradiation. Compared with free resveratrol (RES), the encapsulation of RES into ZPCs (RES-ZPCs) enhanced approximately 5-fold and 2.5-fold antioxidant activity for DPPH and ABTS assays, respectively. Cellular H2O2 scavenging assay of RES-ZPCs presents 100% exogenous reactive oxygen species elimination, whereas free RES eliminates only 63.5%. In vitro cell uptake and cytotoxicity assays show that ZPCs could be uptake and exhibits nontoxic on the cell proliferation. This concept of combining PDA and polyphenols with antioxidant activity and stability may provide new insights into designing highly active, stable polyphenol delivery systems and holds promise for applications in food, dietary supplement, and pharmaceutical industries.