Reversible Supra‐Folding of User‐Programmed Functional DNA Nanostructures on Fuzzy Cationic Substrates

We report that user-defined DNA nanostructures, such as two-dimensional (2D) origamis and nanogrids, undergo a rapid higher-order folding transition, referred to supra-folding, into three-dimensional (3D) compact structures (origamis) or well-defined μm-long ribbons (nanogrids), when they adsorb on soft cationic substrate prepared by layer-by-layer deposition of polyelectrolytes. Once supra-folded, can be switched back the surface their 2D original shape through addition heparin, highly charged anionic polyelectrolyte known an efficient competitor DNA-polyelectrolyte complexation. Orthogonal base-pairing principles, this reversible structural reconfiguration is also versatile; we show in particular 1) it compatible with various origami shapes, 2) perfectly preserves fine details well site-specific functionality, 3) applied dynamically address spatial distribution origami-tethered proteins.