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Formation of ordered mesoporous materials using surfactant templating proceeds via mechanisms relying on optimising interactions between the inorganic and organic components of the synthesis. For oxides, the rates of hydrolysis and condensation of the inorganic species relative the rate of assembly of the mesostructure is crucial. Synthetic strategies to control these factors have been reviewed and it appears that mesostructured silica can be prepared in most phases found in binary surfactant–water systems by optimising the volume fraction of the surfactant and the hydrolysed inorganic precursor.