Topological Single‐stranded DNA Encoding and Programmable Assembly of Molecular Nanostructures for NIR‐II Cancer Theranostics

Abstract Molecular nanotechnology promises to offer privileged access to developing NIR‐II materials with precise structural and functional manipulation for transformable theranostic applications. However, the lack of an affordable, yet general, method makes this goal currently inaccessible. By virtue of the intriguing nucleic acid chemistry, here we present an artificial base‐directed topological single‐strand DNA encoding design that enables one‐step synthesis of valence‐controlled NIR‐II molecular nanostructures and spatial assembly of these nanostructures to modulate their behaviors in living systems. As proof‐of‐concept studies, we construct ultrasmall Ag 2 S quantum dots and pH‐responsive, size‐tunable CuS assemblies for in vivo NIR‐II fluorescence imaging and deep tumor photothermal therapy. This work paves a new way for creating functionally diversified architectures and broadens the scope of DNA‐encoded material engineering.