To fully explore choline amino acid ([Cho][AA]) ionic liquids (ILs) as starch solvents in various applications, the effects of anion structure (reflected from choline lysine ([Cho][Lys])) and choline aspartic acid ([Cho][Asp]) of [Cho][AA]-water solvents on the dissociation and aggregation behaviors of starch were investigated. Compared with water (66.05 °C), the decreased gelatinization temperatures of starch achieved at water/IL (w : IL) ratios of 5 : 5 (64.09 °C) and 4 : 6 (46.96 °C) of [Cho][Lys] solvents indicated the improved dissociation behaviors of starch (also indicated by large values). In contrast, all proportions (w : IL-9:1-2 : 8) of [Cho][Asp] solvents inhibited the dissociation behaviors of starch, leading to increased gelatinization temperatures (above 85 °C). Moreover, after dissolution, the viscosity and