Structural DNA nanotechnology provides unique, well-controlled, versatile, and highly addressable motifs and templates for assembling materials at the nanoscale. These methods to build from the bottom-up using DNA as a construction material are based on programmable and fully predictable Watson-Crick base pairing. Researchers have adopted these techniques to an increasing extent for creating numerous DNA nanostructures for a variety of uses ranging from nanoelectronics to drug-delivery applications. Recently, an increasing effort has been put into attaching nanoparticles (the size range of 1–20 nm) to the accurate DNA motifs and into creating metallic nanostructures (typically 20–100 nm) using designer DNA nanoshapes as molds or stencils. By combining nanoparticles with the superior addressability of DNA-based scaffolds, it is possible to form well-ordered materials with intriguing and completely new optical, plasmonic, electronic, and magnetic properties. This focused review discusses the DNA structure-directed nanoparticle assemblies covering the wide range of different one-, two-, and three-dimensional systems.

DNA origami is used to direct the formation of well-ordered 3D nanoparticle superlattices held together by electrostatic interactions.

Lipids are important building blocks in cellular compartments,a nd therefore their self-assembly into welldefined hierarchicals tructures has gained increasing interest. Cationic lipids and unstructured DNAc an co-assemble into highly ordered structures (lipoplexes), but potential applications of lipoplexes are still limited. Using scaffolded DNA origami nanostructures could aid in resolving these drawbacks. Here,w eh ave complexed DNAo rigami together with ac ationic lipid 1,2-dioleoly-3-trimethylammonium-propane (DOTAP) and studied their self-assembly driven by electrostatic and hydrophobic interactions.The results suggest that the DNAo rigami function as templates for the growth of multilamellar lipid structures and that the DNAo rigami are embedded in the formed lipid matrix. Furthermore,t he lipid encapsulation was found to significantly shield the DNA origami against nuclease digestion. The presented complexation strategy is suitable for aw ide range of DNA-based templates and could therefore find uses in construction of cellmembrane-associated components.

Hierarchical assembly of programmable DNA frameworkssuch as DNA origamipaves the way for versatile nanometer-precise parallel nanopatterning up to macroscopic scales. As of now, the rapid evolution of the DNA nanostructure design techniques and the accessibility of these methods provide a feasible platform for building highly ordered DNA-based assemblies for various purposes. So far, a plethora of different building blocks based on DNA tiles and DNA origami have been introduced, but the dynamics of the large-scale lattice assembly of such modules is still poorly understood. Here, we focus on the dynamics of two-dimensional surface-assisted DNA origami lattice assembly at mica and lipid substrates and the techniques for prospective three-dimensional assemblies, and finally, we summarize the potential applications of such systems.

Cationic phthalocyanines bind DNA origami nanostructures, which protects them against enzymatic degradation and enhances the optical properties of the phthalocyanines.