We present a snapshot of the current status of understanding structure, dynamics, and molecular interactions within deep eutectic solvents (DESs) gained from a computational perspective. The simulations reported thus far have been largely aimed at unravelling the relationship between the molecular features within a DES and the depressed melting temperature at its eutectic composition. Computational efforts consistently reveal that the addition of hydrogen bond, donors significantly disrupts long-range ordering of the cation anion arrangement in choline chloride, resulting in significant moderation of the interaction energies between the components of the DES. These studies paint a picture of DES formation being accompanied by hydrogen-bond directed charge transfer processes yielding transient cage like formation and nanoscale ordering entailing segregation of the ionic and molecular domains. Computational insights further uncover how unique solvation features present within DESs may lead to enhanced biomolecular (e.g., protein, nucleic acid, polysaccharide) stability and/or activity while also offering advantages as environmentally -responsible gas sorbents. (C) 2017 Elsevier B.V. All rights reserved.