The synthesis, characterization, and proposed mechanism of formation of a new family of silicate/aluminosilicate mesoporous molecular sieves designated as M41S is described. MCM-41, one member of this family, exhibits a hexagonal arrangement of uniform mesopores whose dimensions may be engineered in the range of approximately 15 angstrom to greater than 100 angstrom. Other members of this family, including a material exhibiting cubic symmetry, have been synthesized. The larger pore M41S materials typically have surface areas above 700 m2/g and hydrocarbon sorption capacities of 0.7 cc/g and greater. A templating mechanism (liquid crystal templating-LCT) in which surfactant liquid crystal structures serve as organic templates is proposed for the formation of these materials. In support of this templating mechanism, it was demonstrated that the structure and pore dimensions of MCM-41 materials are intimately linked to the properties of the surfactant, including surfactant chain length and solution chemistry. The presence of variable pore size MCM-41, cubic material, and other phases indicates that M41S is an extensive family of materials.