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The physicochemical, rheological properties and structure of potato starch and starch-tea polyphenols (TPs) complex modified by enzyme and alcohol was investigated in this study. Cavities on the modified starch granules and morphology change could be investigated by SEM, while significant birefringence observed in complete granules by polarizing light microscope, but disappeared in crashed starch. TPs inhibited the aggregation of amylose and retrogradation of starch-TPs complex, resulting in the decrease of gel strength, and the increase of viscosity and gelatinization stability of starch granules. Fourier transform infrared (FT-IR) spectra showed that intramolecular hydrogen bond could be formed between TPs with modified starch, and the hydrogen bond force formed by starch and TPs was stronger than that between starch molecules. X-ray diffraction (XRD) analysis revealed that three modification methods did not change the crystalline structure of starch, but new diffraction peaks appeared in the four starch-TPs complex, suggesting that the hydrogen bond was incurred by interaction between TPs and amylose to form V-type crystalline. These results demonstrated that the complex formed by TPs and native/modified potato starch could be used in food industrial applications due to the inhibition of starch retrogradation. • Modified potato starch granules could be prepared with enzyme and alcohol combined with pre-gelatinization. • Modified potato starch granules could adsorb TPs effectively. • The decrease of gel strength, and the increase of viscosity and gelatinization stability of potato starch occurred due to containing the TPs. • Intramolecular hydrogen bond formed between TPs with modified starch molecules, and TPs inhibited the starch-TPs complex retrogradation. • The interaction between TPs and amylose resulted in V-type crystalline of starch granules. [ABSTRACT FROM AUTHOR]