This article provides a brief overview of functional mesoporous silica materials synthesized by the co-structure-directing route, which is distinct from conventional synthesis strategies. In these systems, organosilane serves as the co-structure-directing agent (CSDA), which provides critical interactions between the template and organic part of the organosilane to form mesostructures, thus retaining the organic groups on the pore surface after removal of the template by extraction. i) The formation of anionic-surfactant-templated mesoporous silicas (AMSs) has been achieved by the co-structure-directing route, which leads to a variety of mesostructures, porous properties and morphologies. ii) Other co-structure-directing systems for synthesizing mesoporous silicas have also been achieved, including systems using cationic surfactants and non-surfactants, and systems using DNA for constructing nanofibers and DNA–silica liquid crystalline complexes. iii) Evidence for the regular arrangement of functional groups on the pore surface resulted from the co-structure-directing effect has been discussed. Also included is a brief description of the application, future requirements, and trends in the development of mesoporous materials by the co-structure-directing route.