In this work, the effect of some deep eutectic solvents (DESs) based on choline chloride on water activity (a w ) in aqueous solutions of sucrose was investigated. Activity of water (a w ) and vapor pressure data are obtained precisely using an improved isopiestic technique and correlated with Wilson, e-NRTL, UNIQUAC, and simple polynomial empirical models. The e-NRTL model was successfully employed to calculate the activity coefficient and Gibbs free energies of transfer of sucrose from water to aqueous DES solutions. The results show that the strong interactions between sucrose and the DES are favorable. Also, the Hansen solubility parameters were calculated to predict an appropriate solvent system. The Gibbs free energy results indicate that the salting-in effect is greater in the presence of glycerol-based DES.