Ionic liquids' (ILs) remarkable and tunable physicochemical properties mean they have distinct performance advantages over conventional solvents in many settings. However, the use of ILs in surface-dependent processes (e.g. electrodeposition, heterogeneous catalysis, dye solar cells) is hindered by the lack of a systematic understanding of IL interfacial structure. In this Perspective, we highlight recent experiments which show interfacial IL nanostructure is a consequence of both surface-specific and bulk liquid interactions. These results enable us to develop molecular design rules for controlling interfacial IL behavior.