This review focuses on the synthesis, self-assembled structure and properties of bisurea-based supramolecular polymers. The straightforward synthetic accessibility of the bisurea synthon has allowed the systematic description of the relationship between the molecular structure and supramolecular assembly. Remarkably, these systems self-assemble at equilibrium into two competing supramolecular structures. Therefore, the assembly of low molar mass bisureas can lead to stimuli responsive viscoelastic gels as well as to systems which are able to report on weak intermolecular interactions. When deposited on surfaces, these hydrogen-bonded chains of molecules form well-organized monolayers in spite of defects from the substrate. Moreover, polymers with improved rheological or adhesive properties can be designed by grafting bisurea stickers.