This study presents a symmetry-guided inverse design method for creating self-assembling multiscale DNA origami tilings. The method leverages the symmetries of two-dimensional (2D) tilings to generate interaction matrices that specify the assembly of complex structures. By exploiting the allowed 2D symmetries, the researchers developed an algorithmic approach to generate any periodic 2D tiling from an arbitrarily large number of subunit species, addressing the challenge of engineering 2D crystals with periodicities much larger than subunit size. The method was demonstrated using equilateral triangles synthesized by DNA origami, which were guided to self-assemble into tilings with a wide variety of symmetries using up to 12 unique species of triangles. By conjugating specific triangles with gold nanoparticles, the researchers fabricated gold-nanoparticle supercrystals with lattice parameters spanning up to 300 nm. The study also compares the design economy of various tilings, showing that higher symmetries allow for larger unit cells with fewer subunits, and linear supercrystals can be designed more economically using linear primitive unit cells. The work provides a simple algorithmic approach to designing periodic assemblies, which may enable the multiscale assembly of superlattices of nanostructured "metatoms" with engineered plasmonic functions. The study highlights the importance of symmetry in guiding the self-assembly of complex structures and demonstrates the potential of DNA origami in creating highly ordered, large-scale supercrystals with tunable properties. The results show that the symmetry-based design method is effective in generating complex tilings and supercrystals, and that the design economy can be optimized by considering the symmetry and aspect ratio of the primitive unit cell. The study also discusses the economic cost of synthesizing subunit species and the time required for assembly, highlighting the importance of optimizing these factors for efficient self-assembly. The research has implications for the development of new materials and devices with complex plasmonic and photonic functionalities through self-assembly.This study presents a symmetry-guided inverse design method for creating self-assembling multiscale DNA origami tilings. The method leverages the symmetries of two-dimensional (2D) tilings to generate interaction matrices that specify the assembly of complex structures. By exploiting the allowed 2D symmetries, the researchers developed an algorithmic approach to generate any periodic 2D tiling from an arbitrarily large number of subunit species, addressing the challenge of engineering 2D crystals with periodicities much larger than subunit size. The method was demonstrated using equilateral triangles synthesized by DNA origami, which were guided to self-assemble into tilings with a wide variety of symmetries using up to 12 unique species of triangles. By conjugating specific triangles with gold nanoparticles, the researchers fabricated gold-nanoparticle supercrystals with lattice parameters spanning up to 300 nm. The study also compares the design economy of various tilings, showing that higher symmetries allow for larger unit cells with fewer subunits, and linear supercrystals can be designed more economically using linear primitive unit cells. The work provides a simple algorithmic approach to designing periodic assemblies, which may enable the multiscale assembly of superlattices of nanostructured "metatoms" with engineered plasmonic functions. The study highlights the importance of symmetry in guiding the self-assembly of complex structures and demonstrates the potential of DNA origami in creating highly ordered, large-scale supercrystals with tunable properties. The results show that the symmetry-based design method is effective in generating complex tilings and supercrystals, and that the design economy can be optimized by considering the symmetry and aspect ratio of the primitive unit cell. The study also discusses the economic cost of synthesizing subunit species and the time required for assembly, highlighting the importance of optimizing these factors for efficient self-assembly. The research has implications for the development of new materials and devices with complex plasmonic and photonic functionalities through self-assembly.