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In this study, novel tea polyphenolic-copper hybrid nanoflowers were assembled with tea polyphenol palmitate oligomers generated simply through air oxidation. It was revealed that the growth of tea polyphenolic-based hybrid nanoflowers was notably faster than protein-based ones, presumably owing to rigid polyphenolic molecular architecture and the resultant different growth mechanism. The structures and composition investigation by FT-IR, X-ray, and SEM-EDS unveiled that the whole framework of the nanoflowers was composed of complexes of tea polyphenolic oligomers and copper phosphate crystals. The tea polyphenolic hybrid nanoflowers demonstrated high loading capacity of curcumin due to flower-like porous structure and hydrophobic pockets furnished by lipophilic side chains. The nanoflowers exhibited remarkable protection capacity for carried curcumin from UV irradiation and thermal treatment. Controlled release of the nanoflowers could be readily achieved by adjustment of pH condition. Owing to high assembly efficiency, biocompatibility, and natural abundance, tea polyphenols are intriguing organic components to generate nanoflowers.