Dynamic and reversible assembly of molecules is ubiquitous in the hierarchical superstructures of living systems and plays a key role in cellular functions. Recent work from the laboratory reported on the reversible formation of such superstructures in systems of peptide amphiphiles conjugated to oligonucleotides and electrostatically complimentary peptide sequences. Here, a supramolecular system is reported upon where exchange dynamics and host-guest interactions between -cyclodextrin and adamantane on peptide amphiphiles lead to superstructure formation. Superstructure formation with bundled nanoribbons generates a mechanically robust hydrogel with a highly porous architecture that can be 3D printed. Functionalization of the porous superstructured material with a biological signal results in a matrix with significant in vitro bioactivity toward neurons that could be used as a supramolecular model to design novel biomaterials.

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Multiple metastable doubly threaded [3]rotaxanes using a large 46 atom ring were prepared and fully characterized. Varying the stopper group size gave a range of interlocked stabilities in CDCl3 from a half-life of <1 minute to ca. 6 months.

The self‐assembly of small molecules into supramolecular polymers can be analogous to the formation of classical solid‐state crystals depending on the mechanism of polymerization. Taking inspiration from the field of materials science, complex supramolecular polymer nanostructures can be formed by carefully controlling nucleation and growth processes. Exploration of the energy landscapes in supramolecular polymers can also lead to the discovery of polymorphs where a single monomer can self‐assemble into different supramolecular polymers with distinct molecular packing arrangements. This mini‐review focuses on recent developments where the manipulation of nucleation and growth processes were used to develop novel supramolecular copolymers and explore polymorphism in supramolecular materials, highlighting examples of such systems composed of small organic molecules and peptides. © 2022 The Authors. Polymer International published by John Wiley & Sons Ltd on behalf of Society of Industrial Chemistry.