Understanding how organic molecules interact with water is crucial in fields like health care and medication , synthetic chemistry 2 , environmental chemistry , and renewable energy, etc. The hydration modifies the solvent bonding network and the solution properties. Hydration of small-sized molecules such as methanol, tetrahydrofuran results in the binary aqueous systems performing differently from the pristine water or the organic solutes, such as protein solubility, chemical reactivity, elastoviscosity, surface stress, freezing point, electric and heat conductivity, etc ; Hydration of macromolecules, such as deoxyribonucleic acids and proteins, affects the formation of the heterogeneous assemblies and essential biological functions. As a result, the versatile binary mixtures have found wide-reaching applications serving as cryoprotectants, cosolvents, clathrates, and electrolytes , etc. However, little is yet known about the type and dynamical relaxation of the intra-solute and hydration interfacial interactions.