Some examples of the use of molecular dynamics simulation to study solutions of small molecules in ionic liquids are discussed. It is shown that electrostatic forces, while not the dominant solute–solvent interaction, determine the local solute environment. The solubility of aromatics and the changes in the spectra of low-frequency intermolecular vibrations in two related ionic liquids (one dicationic and one monocationic) are compared with experimental results and related to the local environment.