Programmable Cocrystallization of DNA Origami Shapes

Assembly of distinct types of species, particularly possessing anisotropic configurations, is the premise to broaden structural diversity and explore materials' collective properties. However, it remains a great challenge to programmably cocrystallize manifold anisotropic nanoparticles with the desired assembly mode, because it requires not only the complementarity of both sizes and shapes but also the control over their directional interactions. Here, by introducing DNA origami technique into lattice engineering, we synthesize two types of DNA nano-objects with different symmetries and program the heterogeneous functional patches precisely on their surfaces with nanometer-level precision, which could guide further assembly of these nano-objects. We show that these anisotropic DNA nano-objects could be cocrystallized along specified modes via modulating the combination of surface patches. The highly ordered DNA crystals were thoroughly evidenced by techniques including small-angle X-ray scattering and electron microscopy after careful encapsulation of a thin layer of silica on these DNA nano-objects. Our strategy endows distinct shapes of organic DNA origami structures with regulation features to control the sophisticated modes of cocrystallization of these diverse components, laying a foundation for designing and fabricating customized three-dimensional structures with given optical and mechanical properties.