Nanostructured materials have many forms. One that has been somewhat neglected until recently is organogels, especially those whose three-dimensional structural networks are based on the self-assembly of low molecular-mass organic gelators (LMOGs). These thermoreversible materials consist of a small amount of LMOG and an organic liquid. Because of the wide diversity of structures of molecules known to function as LMOGs and the dearth of direct information concerning how they pack in their gel assemblies, it has been difficult to decipher the salient features that constitute an LMOG. The stepwise simplification of LMOG structures and the development of methods to determine their packing in organogels at the micrometer-to-angstrom distance regimes are discussed for the simplest known LMOGs to the more complex, such as CEP (see Figure), which is known to form molecular wires when gelling chloroform. Work from the laboratory of the authors is emphasized. In addition, an overview of current and potential applications for these materials is presented.