A central goal in nanotechnology is to create structures with precise control over both structural and chemical features. DNA has proven to be an excellent building block for nanoscale materials, due the programmability of Watson-Crick pairing and well-characterized structural properties. However, DNA nanostructures lack the chemical and physical diversity of proteins, and as nanoscale scaffolds they are constrained by the geometric parameters of the B-form duplex. Here, we integrated a programmable protein-derived motif, the coiled-coil, with DNA nanostructures to create hybrid materials that merge both self-assembling units. A heterodimeric coiled-coil peptide pair, synthesized by solid-phase peptide synthesis, was attached to two different DNA handles using strain-promoted azide-alkyne cycloaddition. These handles allowed the coiled coil to be integrated with DNA origami, for the formation of extended 1D arrays driven by the peptide interactions. We explored several mechanisms of self-assembly, including both one-pot and two hierarchical methods. We then extended this approach to two orthogonal pairs of coiled-coils, and used this system to assemble nanofibers that integrate proteins. A bioactive domain from fibronectin was fused with two peptides, and used as a linker to assemble DNA-peptide nanostructures into 1D arrays. We foresee that these materials will serve as novel biomaterials that merge the programmability of DNA with the structural and functional diversity of peptide motifs, and greatly expand the toolkit of biomolecular nanotechnology.

Hybrid nanomaterials through the self-assembly of coiled-coil peptides and DNA nanostructures

ACS Spring Meeting 2021

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