Pyramidal molecular hosts related to cyclotriveratrylene (CTV) form self-assembled cages including organic cages, hydrogen-bonded cages, and metallocages. The latter include M3L2, M4L4, M6L8, and M12L8 assemblies, including topologically complicated structures. Metallocages may show ligand exchange and/or homochiral sorting of the C-3-symmetric CTV-analog ligands. Cages also occur within coordination networks.