At low temperatures, liquid crystal-like arrays made up of inorganic-cluster and organic molecular units readily undergo reversible lyotropic transformations. Gemini surfactants, with two quaternary ammonium head groups separated by a methylene chain of variable length and with each head group attached to a hydrophobic tail, can be used to control organic charge sitting relative to the bivariable hydrophobic tail configurations. This approach has led to the synthesis of a mesophase (SBA-2) that has three-dimensional hexagonal (P6(3)/mmc) symmetry, regular supercages that can be dimensionally tailored, and a large inner surface area. This mesostructure analog of a zeolite cage structure does not appear to have a lyotropic surfactant or lipid liquid crystal mesophase counterpart. Through the modification of gemini charge separation and each of the two organic tails, these syntheses can be used to optimize templating effects, including the synthesis of MCM-48 at room temperature.