DNA Hybridization Tunes Hierarchical Assembly of Supramolecular Copolymers

In nature, the reversible supramolecular organization of biomolecules from the nanoscale to the macroscale creates functional structures that regulate key biological processes. Howvere, it remains challenging to tune hierachical assembly in synthetic analogs. Here, we report on DNA-decorated supramolecular brush nanofibers, where DNA base-pairing drives the hierarchical assembly of the peptide-DNA brush nanofibers. We tune hierarchy in the peptide-DNA material by designing peptide-DNA duplexes with varying stability and junction type. We also tune the reconfiguration of the material by controllably disrupting the amount of DNA hybridization between brush fibers using a chemical trigger. Finally, we demonstrate how this biomolecular reconfiguration can be used for the incremental release of a protein payload. This peptide-DNA platform provides a way to tune both hierarchical morphologies and stimuli responsiveness through material design.