This tutorial review reports upon the organisation and functionalization of two families of hybrid organic–inorganic materials. We attempted to show in both cases the best ways permitting the organisation of materials in terms of properties at the nanometric scale. The first family concerns mesoporous hybrid organic–inorganic materials prepared in the presence of a structure-directing agent. We describe the functionalization of the channel pores of ordered mesoporous silica, that of the silica framework, as well as the functionalization of both of them simultaneously. This family is currently one of the best supports for exploring polyfunctional materials, which can provide a route to interactive materials. The second family concerns lamellar hybrid organic–inorganic materials which is a new class of nanostructured materials. These materials were first obtained by self-assembly, as a result of van der Waals interactions of bridged organosilica precursors containing long alkylene chains during the sol–gel process, without any structure directing agent. This methodology has been extended to functional materials. It is also shown that such materials can be obtained from monosilylated precursors.