Over the last decade, DNA origami has matured into one of the most powerful bottom-up nanofabrication techniques. It enables both the fabrication of nanoparticles of arbitrary two-dimensional or three-dimensional shapes, and the spatial organization of any DNA-linked nanomaterial, such as carbon nanotubes, quantum dots, or proteins at ∼5-nm resolution. While widely used within the DNA nanotechnology community, DNA origami has yet to be broadly applied in materials science and device physics, which now rely primarily on top-down nanofabrication. In this article, we first introduce DNA origami as a modular breadboard for nanomaterials and then present a brief survey of recent results demonstrating the unique capabilities created by the combination of DNA origami with existing top-down techniques. Emphasis is given to the open challenges associated with each method, and we suggest potential next steps drawing inspiration from recent work in materials science and device physics. Finally, we discuss some near-term applications made possible by the marriage of DNA origami and top-down nanofabrication.