The small-angle neutron scattering (SANS) and dynamic light scattering (DLS) investigation were carried out for organogels in toluene, formed by organogelators, to elucidate the relationship between the chemical structure and the gelation mechanism as well as the physical properties of the gels. Three different organogelators, that is cyclo(L-beta-3,7-dimethyloctylasparaginyl-L-phenylalanyl) (CPA), trans(1R,2R)-bis(undecylcarbonylamino)cyclohexane (TCH), and N-epsilon-lauroyl-N-alpha-stearylaminocarbonyl-L-lysine ethyl ester (LEE), were chosen for comparison. The SANS intensity functions of toluene solutions of these gelators could be reduced with the concentration and were described with a scattering function for thin rods. This indicates that the gels consist of noncorrelated, rod-like elements aggregated to each other. The characteristic features of the gelation properties, such as the critical gelation concentration, C-gel, the gelation temperature, T-gel, the gel structure, and the gelation mechanism, were different from each other. CPA had the lowest Cgel and became a gel gradually as the temperature decreased, while TCH and LEE had higher C(gel)s and underwent a sharp sol-gel transition. We conclude that the gelation mechanisms between the CPA and TCH solutions are different. The "CPA type" gelators form a gel by a linear extension of hydrogen-bonded plane, while the "TCH type" gelators form a twisted wire, because of its strong helicity and crystallizability. In addition, in the latter type, a next generation of fibrils easily stacks on top of the previous ones to form larger fibrils. These models well explain the DLS results and the mechanical properties. That is, the fibrillar stems in CPA gels are rather mobile and fragile, while those in TCH and LEE are frozen and brittle. (c) 2005 Wiley Periodicals, Inc.