As a class of materials, supramolecular polymers represent an exciting area of advanced materials research. The combination of unique properties, easy synthesis and response to the environment or external and temporal stimuli makes them important as a focus for the next generation of materials. Understanding and manipulating the non-covalent interactions leading to polymer assembly allows control over properties by selecting specific building blocks with well-understood non-covalent chemistry from an established toolkit. This allows assembly of defined and easily manipulated architectures, where physical characteristics similar to conventional high-molecular-weight polymers can be realized. Herein, we describe recent studies of the self-assembly of polyurethane-based supramolecular materials.