Constructing high‐order DNA nano‐architectures in large sizes is of critical significance for the application of DNA nanotechnology. Robust and flexible design strategies together with easy protocols to construct high‐order large‐size DNA nano‐architectures remain highly desirable. In this work, the authors report a simple and versatile one‐pot strategy to fabricate DNA architectures with the assistance of spherical gold nanoparticles modified with thiolated oligonucleotide strands (SH‐DNA‐AuNPs), which serve as “power strips” to connect various DNA nanostructures carrying complementary ssDNA strands as “plugs”. By modulating the plug numbers and positions on each DNA nanostructure and the ratios between DNA nanostructures and AuNPs, the desired architectures are formed via the stochastic co‐assembly of different modules. This SH‐DNA‐AuNP‐mediated plug‐in assembly (SAMPA) strategy offers new opportunities to drive macroscopic self‐assembly to meet the demand of the fabrication of well‐defined nanomaterials and nanodevices.

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In recent decades, DNA nanotechnology has grown into a highly innovative and widely established field. DNA nanostructures have extraordinary structural programmability and can accurately organize nanoscale materials, especially in guiding the synthesis of metal nanomaterials, which have unique advantages in controlling the growth morphology of metal nanomaterials. This review started with the evolution in DNA nanotechnology and the types of DNA nanostructures. Next, a DNA-based nanofabrication technology, DNA metallization, was introduced. In this section, we systematically summarized the DNA-oriented synthesis of metal nanostructures with different morphologies and structures. Furthermore, the applications of metal nanostructures constructed from DNA templates in various fields including electronics, catalysis, sensing, and bioimaging were figured out. Finally, the development prospects and challenges of metal nanostructures formed under the morphology control by DNA nanotechnology were discussed.