Different intermolecular interactions are involved in the multiscale hierarchical self-assembly of peptides. Different intermolecular interactions have distinct roles for the hierarchical self-assembly process stepping at different scales, from elementary molecules to secondary structures such as β-sheets and α-helices, to fibres and fibre bundles, and even to crystalline structures. It should be noted that intermolecular β-sheets and helices are often formed in short peptide self-assembly, whereas intramolecular sheets and helices can be formed in polypeptide and protein self-assembly. Reproduced with permission from REF.156, Wiley-VCH.