Abstract
Structural DNA nanotechnology makes the programmable design and assembly of DNA building blocks into user-defined microstructures feasible. However, the formation and further growth of these microstructures requires slow heat treatment in precise instruments, as otherwise amorphous aggregates result. Here, we used an organic solute, urea, as the catalyst for the crystallization of DNA origami building blocks to achieve the fast synthesis of DNA origami single crystals with a cubic Wulff shape at room temperature. The ordered assemblies can be formed within 4 hours at room temperature, which further grew into cubic microcrystals with an average size of about 5 micrometers within 2 days. Furthermore, the phase diagram provides an inverse logic that allows users to proactively customize the melting temperature (T (m)) of crystallization according to the target temperature conditions, rather than requiring de novo design of DNA sequences or painstakingly difficult trial-and-error attempts. On this basis, even under random fluctuating outdoor temperature conditions, DNA origami crystals can still grow and maintain high quality and high yield comparable to those of crystals synthesized in precise instruments, creating a basis for the development of adaptive self-assemblies and the industrialization of functional DNA microstructures.