The rheological and adhesive properties of bis‐urea functionalized low‐molecular‐weight polyisobutylenes (PIBUT) are investigated. The polymers, which can interact through supramolecular hydrogen bonds, can self‐organize over times of the order of days at room temperature. This organized structure has been identified by small angle X‐ray scattering (SAXS) and its rheological properties indicate the behaviour of a soft viscoelastic gel. The ordered structure can be disrupted by temperature and shear so that at 80 °C, the material behaves as a highly viscoelastic fluid and no SAXS peak is observed. When cooled back at room temperature, the PIBUT retrieves its ordered structure and gel properties after 20 h of annealing. This very slow molecular dynamics gives PIBUT a highly dissipative nature upon deformation, which combined with strongly interacting moieties results in very interesting adhesive properties both on steel surfaces but more importantly on typical low adhesion surfaces such as silicone. A strategy based on the controlled incorporation of supramolecular bonds in a covalently crosslinked network appears promising for the development of a new generation of highly interacting and dissipative soft adhesives.

The mechanical and adhesive properties of a series of model nanostructured waterborne PSA films have been characterized. The base polymer composition of the latex has been kept constant but systematic modifications have been carried out: the introduction of nanoparticles localized at the interfaces between particles, and the incorporation of a crosslinking agent. The mechanical properties have been characterized and show that the most effective modifications result in an increase in the low‐frequency modulus in the small‐strain regime and in a more pronounced softening and strain‐rate‐dependent behavior in the large‐strain regime. In industrial standard tests, this combination gives a dramatically increased resistance to shear while maintaining a high value of peel resistance. magnified image