“…13–16 Peptide assemblies are ordinarily governed by a combination of noncovalent and covalent interactions, encompassing hydrogen bonds, 17 π–π stacking, 18 hydrophobic interactions, 19,20 coulombic forces, 21,22 disulfide S–S bonds, 23,24 l -phenylalanine polymerization, dityrosine crosslinking, 25–27 and so on, which could drive peptide self-assembly processes, stabilize secondary or tertiary structures, and establish conjugation patterns even at the protein level. Tremendous efforts have been made to exploit de novo designed peptides and mimic bioactive assemblies, however, the function-oriented synthesis is still limited by many influencing factors of pH environment, 28–30 working temperature, 31–33 ionic strength, 34,35 hydrophilic/hydrophobic properties, 36,37 pre-assembly method, 38,39 host–guest modeling, 40,41 spacer occupation, 42,43 and so on.…”