Read the full paper here: Nano Letters, doi:10.1021/acs.nanolett.6b04146 (2016). The rational design of anisotropic interaction patterns is a key step for programming colloid and nanoparticle self-assembly and emergent functions. Herein, we demonstrate a concept for harnessing the capabilities of 3D DNA origami for extensive supracolloidal self-assembly, and showcase its use for making truly monodisperse, patchy, divalent nanocuboids that can self-assemble into supracolloidal