We report on the self‐assembly in water of a set of bis‐urea amphiphiles. A range of techniques, including dynamic light scattering, Cryo‐TEM, SAXS, and MS are used to study the effect of structural variation on the morphology of the assemblies. The length, dispersity, and end‐group of the ethylene glycol hydrophilic part of the molecule, as well as of the alkyl chain length are varied to tailor the morphology towards soluble wormlike micelles. Slight modification on molecular structures gave a large difference in self‐assembly behavior in water, giving guidelines for the design of rodlike supramolecular fibers with novel functionalities, such as strain‐stiffening and bioactivity.