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Hierarchical peptide assembly has yielded a rich array of functional materials and adaptive matter. This special issue explores recent advances in the synthesis of well‐defined peptide structures and their utilization as biomaterial scaffolds. Among these, non‐canonical amino acids have evoked particular interest due to their ability to produce de novo peptides with unique bioactivities. Medina and co‐workers describe how fluorinecontaining amino acids have been incorporated into peptides and proteins to evolve an entirely new class of biomolecular building blocks. By exploiting the fluorous effect to drive assembly, these non‐natural sequences have catalyzed the construction of biomaterials with diverse supramolecular morphologies. (doi: 10.1002/pep2.24184 )