Hierarchical Assembly of Multilayer Core-Shell DNA Origami Crystals.

A multilayer core-shell architecture capable of selectively capturing distinct nanomaterials into a predetermined layer is anticipated to facilitate multifunctional isolation or cascade processes at the microscale. However, fabricating single-crystal architectures featuring numerous shells with intricate distribution patterns remains challenging. In this study, we employed DNA nanotechnology to construct microscale multilayer core-shell DNA origami crystals. The internal layers exhibit tunable properties, including size, quantity, self-similarity, and morphology. The shell size can be regulated from 700 to 1800 µm3, and the layer quantity can be extended to five. We also fabricated eight distinct crystals exhibiting non-self-similarity and two types of heteromorphic core-shell crystals. Each layer has operational independence, allowing the customized capture of nanomaterials and implementation of compartmentalized reactions. These multilayer core-shell crystals have potential for serving as compartmentalization templates for functional units, which may provide possibilities for simulating cell work or constructing artificial organelles.