Starch is a clean-label food ingredient, yet its applications in its native form are limited. The linear components of starch, including amylose and the linear side chains of amylopectin, can form inclusion complexes (ICs) with various guest molecules, significantly changing the structure and functional properties of starch. Meanwhile, the stability of encapsulated bioactive compounds can be improved. In this study, structural transformations of starch were investigated to establish starch as a versatile carrier for bioactive compounds with tunable digestion behavior. High-amylose corn starch (amylose content ≈72%) was first dissociated in solvent, converting its original crystalline structure into an amorphous state. Subsequent annealing in aqueous ethanol reshaped the starch into a V-type crystalline structure composed of single helices, with ethanol concentration and temperature serving as key parameters for fine-tuning structural formation, as confirmed by X-ray diffraction analysis. The resulting helical structures were then used as carriers for curcumin loading via thermal treatment in aqueous ethanol, with 40% ethanol yielding the highest loading capacity. Encapsulated curcumin exhibited enhanced water dispersibility and color stability compared to its free form. This approach provides a promising strategy for designing functional food systems with improved water dispersibility of the hydrophobic pigments and stability of sensitive bioactive compounds.