A coassembly methodology was developed to synthesize ordered mesoporous silica materials containing gold nanoparticles. The essence of this methodology lies in the combination of the complexation-mediated growth of nanoparticles and surfactant-templating synthesis. The formation of nanoparticles was controlled by the complexing ligand and the unique micellar media. Different methods for the removal of the templating surfactants were evaluated. Ordered mesoporous silica materials containing 2-5 nm gold nanoparticles have been successfully synthesized.