Heteroleptic metal−organic capsules, which incorporate more than one type of ligand, can provide enclosed, anisotropic interior cavities for binding low-symmetry molecules of biological and industrial importance. However, the selective selfassembly of a single mixed-ligand architecture, as opposed to the numerous other possible self-assembly outcomes, remains a challenge. Here, we develop a design strategy for the subcomponent self-assembly of heteroleptic metal−organic architectures with anisotropic internal void spaces. Zn 6 Tet 3 Tri 2 triangular prismatic and Zn 8 Tet 2 Tet′ 4 tetragonal prismatic architectures were prepared through careful matching of the side lengths of the tritopic (Tri) or tetratopic (Tet, Tet′) and panels.