A large family of amphiphilic pseudopeptidic derivatives in which the aliphatic tails are connected to the pseudopeptidic moiety through urea functionalities have been prepared with excellent yields. The synthetic procedure is simple and very efficient and allows a modular variation of a large number of structural parameters. The self-assembling properties of the resulting compounds has been studied under different conditions and using different media. Very interestingly, many of the compounds obtained have revealed to act as very efficient organogelators at low concentrations. The resulting gels provide some unusual properties. Of particular relevance are the broad scope of organic solvents that can be gelated and the high thermal stability of the resulting gels. Gels that are stable up to temperatures close to 100 °C can be obtained in some instances.