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In this study, amylose, known as the food-grade biopolymers has been proved as a feasible solution for the controlled delivery of quercetin. The effect of reaction variables including reaction temperature, time, pH and quercetin addition amount on the content and conversion rate of quercetin was analyzed. Meanwhile, fourier transform infrared spectroscopy (FT-IR) and X-ray diffraction (XRD) provided evidence of quercetin complexation with amylose. Then, the molecular, cluster, and fractal structures of the complexes were investigated using 13C cross-polarization/magic angle spinning nuclear magnetic resonance (13C CP/MAS NMR) and small-angle X-ray scattering (SAXS). Furthermore, laser scanning confocal microscopy (CLSM) identified the precise encapsulation structure from direct observation and scanning electron microscope (SEM) was conducted to show that complexes displayed a larger size granule with smooth and angular appearance. From the antioxidant study, amylose/quercetin complexes presented effective scavenging capacity toward DPPH•. Besides, complexes showed high retention of quercetin in simulated stomach conditions but gradual release in simulated small intestine conditions. It was therefore confirmed that the amylose/quercetin complexes could be served as suitable carriers for the controlled release of quercetin in the digestive tract. The present research expanded the application range of starch, meanwhile proved an alternative application prospect for the ameliorative bioactive quercetin products. [ABSTRACT FROM AUTHOR]