A neutral templating route for preparing mesoporous molecular sieves is demonstrated based on hydrogen-bonding interactions and self-assembly between neutral primary amine micelles (S degrees) and neutral inorganic precursors (I degrees). The S degrees I degrees templating pathway produces ordered mesoporous materials with thicker framework walls, smaller x-ray scattering domain sizes, and substantially improved textural mesoporosities in comparison with M41S materials templated by quaternary ammonium cations of equivalent chain length. This synthetic strategy also allows for the facile, environmentally benign recovery of the cost-intensive template by simple solvent extraction methods. The S degrees I degrees templating route provides for the synthesis of other oxide mesostructures (such as aluminas) that may be less readily accessible by electrostatic templating pathways.