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Although a variety of DNA‐based molecular machines had already been realized before the invention of the scaffolded DNA origami method [18–21], its excellent shape designability [12, 22, 23] brought remarkable progress in the development of DNA nanodevices and DNA nanorobots [24]. Representative examples include a nano‐sized box capable of being opened by reacting with a specific “key” DNA strand [25], pH‐ or photoresponsive nanocapsules [26, 27], and a capsule‐shaped nanorobot that recognizes specific proteins on the specific cell surface to expose its cargos [28]. In addition to these container‐like structures, researchers have attempted to imitate normal‐sized mechanical parts, such as bearings, sliders, and hinges with DNA origami [29–31]. Coordinated operations that combine multiple mechanical units have also been examined [30]. These mechanical motions are often regulated by strand displacement reactions [18], DNAzyme‐mediated cleavage [32], triplex formations [27], and quadruplex formations such as a guanine quadruplex (G‐quadruplex) and i‐Motifs [29, 33]. It is noteworthy that all of these can, in principle, be realized with natural nucleobases, exhibiting the great advantages of DNA as a material that not only enables the design of arbitrarily shaped nanostructures but also allows us to design responses to stimuli such as ions, pH changes, or small molecules, using only four fundamental nucleotides.