Enzyme-triggered hydrogelation via self-assembly of alternating peptides

α-Chymotrypsin catalyzed oligomerization of the “dipeptide lego” KL-ethyl ester (OEt) in aqueous media triggers a rapid sol–gel transition due to formation of alternating (KL)x. Resulting mixed chain oligomers, at alkaline pH, self-assemble into β-sheets. Thereafter, intermolecular backbone hydrogen bonding between peptides causes formation of physically entangled nanofibrillar networks.