Programming One‐Dimensional Open‐Channel Superlattices with Edge‐Bonding of Meta‐DNA

Abstract The physicochemical properties of one‐dimensional (1D) porous nanomaterials are fundamentally influenced by their channel geometrical and topological characteristics. However, synthesis of geometrically and topologically diversified 1D porous crystals spanning the mesoporous‐to‐macroporous range remains a significant challenge. Here, we present a universal strategy for constructing 1D open‐channel superlattices through edge‐to‐edge assembly (edge‐bonding) of DNA‐sparsely modified meta‐DNA (M‐DNA). By programming the rigidity and length of sparsely distributed DNA bonds on M‐DNA surfaces, we achieved long‐range ordered assembly of triangular M‐DNA 1D single‐channel superlattice (3.7 ± 1.2 µm) with a macroporous structure. The generality of this approach was further demonstrated by assembling hexagonal M‐DNA into 1D multi‐channel superlattice (3.6 ± 1.0 µm) with a mesoporous structure, thereby reducing the pore size from 140 to 29 nm and the porosity from ∼94.2 to ∼87.5%. Furthermore, an ultrathin gold layer grown on the triangular M‐DNA superlattice exhibited a ∼3.3‐fold enhancement in electrocatalytic activity compared to non‐assembled triangular M‐DNA, attributed to the increased surface area and narrower bandgap. This work broadens the design framework for porous crystals assembled via DNA nanotechnology and highlights their potential applications in catalysis, energy conversion, and beyond.