The crystal and molecular structures of [Me(2)Etim]Cl, [Me(2)Etim](2)[CoCl4], and [Me(2)Etim](2)[NiCl4] ([Me(2)Etim](+) = 1,2-dimethyl-3-ethylimidazolium cation) all contain evidence that the H4 and H5 protons of the imidazolium cation enter into hydrogen bonds; the implications of this observation for the interactions in room-temperature chloroaluminate(III) ionic liquids are considered.