Environment-Resistant DNA Origami Crystals Bridged by Rigid DNA Rods with Adjustable Unit Cells.

The crystallization methodology of DNA origami frames has found salient utility in large-scalely integrating multifarious functional components following organized arrangements, thus opening up the possibilities for optical, biological, and other interdisciplinary applications. However, the single strand-dominated spacing region between adjacent DNA origami units has extremely restricted the adjustment of DNA origami separations, leading the soft crystals susceptible to environmental influences. Herein, we developed a cocrystallization pathway by incorporating rigid DNA rods into a DNA origami assembly system to achieve mutually ordered bridging on a three-dimensional scale. The intervention of DNA rods significantly improved the rigidity and crushing resistance of entire cocrystals and rendered DNA origami units exhibiting different spacing distances within the obtained crystal phase when varying DNA rod structures artificially. Such a tuning strategy that uses DNA rods as allosteric factors would provide a rational method for accessing diverse crystalline states and even modulating the tailorable properties of materials on demand.