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DNA origami technology enables the precise assembly of well-defined two-dimensional and three-dimensional nanostructures with DNA, an inherently biocompatible material. Given their modularity and addressability, DNA origami objects can be used as scaffolds to fabricate larger higher-order structures with other functional biomolecules and engineer these molecules with nanometer precision. Over the past decade, these higher-order functional structures have shown potential as powerful tools to study the function of various bio-objects, revealing the corresponding biological processes, from the single-molecule level to the cell level. To inspire more creative and fantastic research, herein, we highlight seminal works in four emerging areas of bioapplications of higher-order DNA origami structures: (1) assisting in single-molecule studies, including protein structural analysis, biomolecule interaction analysis, and protein functional analysis, (2) manipulating lipid membranes, (3) directing cell behaviors, and (4) delivering drugs as smart nanocarriers. Finally, current challenges and opportunities in the fabrication and application of DNA origami-based functional structures are discussed. This review highlights the recent advances in the bioapplications of higher-order DNA origami structures at multiple scales. After a brief introduction to the development of DNA origami, we describe the use of DNA origami structures to assist in single-molecule studies, manipulate lipid membranes, direct cell behaviors, and deliver drugs as smart nanocarriers. Our opinions on the current challenges and future directions are also shared. [ABSTRACT FROM AUTHOR]

Herein, we report the assembly of gold nanobipyramids (AuNBPs) into static and dynamic chiral plasmonic nanostructures via DNA origami. Compared with conventional chiral dimers of gold nanorods (AuNRs), AuNBP dimers exhibit more intriguing chiroptical responses, suggesting that they could be a superior alternative for constructing chiral plasmonic nanostructures for biosensing. [ABSTRACT FROM AUTHOR]

Self‐assembled plasmonic logic gates that read DNA molecules as input and return plasmonic chiroptical signals as outputs are reported. Such logic gates are achieved on a DNA‐based platform that logically regulate the conformation of a chiral plasmonic nanostructure, upon specific input DNA strands and internal computing units. With systematical designs, a complete set of Boolean logical gates are realized. Intriguingly, the logic gates could be endowed with adaptiveness, so they can autonomously alter their logics when the environment changes. As a demonstration, a logic gate that performs AND function at body temperature while OR function at cold storage temperature is constructed. In addition, the plasmonic chiroptical output has three distinctive states, which makes a three‐state molecular logic gate readily achievable on this platform. Such DNA‐based plasmonic logic gates are envisioned to execute more complex tasks giving these unique characteristics. [ABSTRACT FROM AUTHOR]