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The presence of water or Methanol in ionic liquids has a large effect on physical properties. There are a number of papers, which have studied the physical properties of binary systems of ionic liquids . However, few reports related to the structures and the AAILs mixtures interactions of AAILs at theoretical level have been found, the mechanism of the cation–anion interaction for AAILs has not been fully understood. It is necessary to investigate these interaction systems systematically by theoretical or experimental methods. Among various experimental techniques, infrared spectroscopy is a convenient and effective approach for the study of H-bonding interactions at the molecular level. In this paper, the structures and interactions of the [bmim][Ala], [bmim][Ala] and water /Methanol have been systematically studied by density functional theory, the ATR-IR spectra of the [bmim][Ala], [bmim][Ala] and water /Methanol were investigated. The results will be helpful for understanding of these AAILs from the perspective of structure and the AAILs mixtures interactions, and it could provide some important information for the continuous exploitation and application of AAILs.