Recent advances in the design and synthesis of mesostructured and mesoporous materials with nonoxide frameworks are reviewed. Chalcogenides comprise the most important class, and all possible pore arrangements known for silica can be achieved in these materials. The special molecular chemistry that leads to organized nonoxidic mesostructures that have a variety of compositions, pore sizes, and semiconductor bandgaps is presented. Also reviewed are recent developments in mesoporous elements, such as metals and germanium. The goal in research on mesoporous semiconductors is to create materials scaffolds with new physical phenomena that derive from the combined characteristics of long-range porosity and electronic and optical properties.