LAUSR

Significance This paper reports an exciting breakthrough in dynamic biomaterials design mimicking the reversible interlocking and remoldable structure of extracellular matrix (ECM). Specifically, we realize a nature-derived molecular recognition event (i.e., the antibiotic glycopeptide vancomycin [Van] and the dipeptide d-Ala-d-Ala [AA] receptor–ligand interaction) as a reversible strategy for fabrication of dynamic biointerface and 3D ECM mimics. We believe that the specific but reversible Van–AA molecular recognition would be a strategy for dynamic biomaterial fabrication, and that the easy-handling merit, ECM-like remoldability, and inherent antibacterial activity will bring insights to biomaterial scaffold design in tissue engineering and regenerative medicine. Dynamic biomaterials excel at recapitulating the reversible interlocking and remoldable structure of the extracellular matrix (ECM), particularly in manipulating cell behaviors and adapting to tissue morphogenesis. While strategies based on dynamic chemistries have been extensively studied for ECM-mimicking dynamic biomaterials, biocompatible molecular means with biogenicity are still rare. Here, we report a nature-derived strategy for fabrication of dynamic biointerface as well as a three-dimensional (3D) hydrogel structure based on reversible receptor–ligand interaction between the glycopeptide antibiotic vancomycin and dipeptide d-Ala-d-Ala. We demonstrate the reversible regulation of multiple cell types with the dynamic biointerface and successfully implement the dynamic hydrogel as a functional antibacterial 3D scaffold to treat tissue repair. In view of the biogenicity and high applicability, this nature-derived reversible molecular strategy will bring opportunities for malleable biomaterial design with great potential in biomedicine.