Low molecular weight gelators, LMWG, are small molecules that can self-associate in organic solvents or in water to form fibrous supramolecular architectures and three-dimensional networks that present important applications in several fields. Although various strategies are known for the synthesis of this type of compounds, these are commonly hampered by the use of long multi-step processes that include the protection and deprotection of functional groups. Therefore, it is essential to find direct and robust reactions that allow the simple and efficient introduction of complexity and structural diversity. A promising approach to this end is the use of multicomponent reactions. Based in our experience in this field, here we report our studies aimed at the use of multicomponent reactions of isocyanides to prepare low molecular weight gelators.