Macroscopic assembly of centimeter-scale monolayer two-dimensional DNA origami polymers

The construction of macroscopic, hierarchically ordered macroscopic superstructures from nanoscale building blocks remains a fundamental challenge in materials science. DNA origami provides a powerful platform for achieving high-precision organization, yet the translation of its programmability to macroscopic dimensions has been hindered by weak interaction energies and slow kinetics at larger scales. Here, we report macroscopic assembly of centimeter-scale, free-standing monolayer films of two-dimensional DNA origami polymers (2D-DOPs) using a surfactant-mediated interfacial assembly strategy. Using a tailored surfactant (Dioctyl sodium sulfosuccinate, DSS) which provides a high interfacial activity and a surface tension reduction of 36.0 mN/m in the buffer solution, we achieve highly coherent 2D-DOP films with single-crystalline domains up to 1,200 μm². We find that the fluid surfactant matrix effectively enhances interfacial mobility, enabling DNA origami monomers to overcome kinetic traps in solution. These films can be chemically modified, silicified and transferred to arbitrary substrates, which reveals a pronounced photonic bandgap in the deep ultraviolet region. This approach is generalizable across diverse origami geometries, allowing arbitrary pattern design, and establishes a scalable route for producing 2D macroscopic materials from DNA-based nanoscale building blocks.