This paper reports on hybrid organic-inorganic dense membrane materials in which protons and ions are envisioned to diffuse along the hydrophilic pathways. The hierarchical generation of functional hybrid materials was realised in two steps. First, the self-assembling properties of 3-(ureidoarene)propyltriethoxysilane compounds 1-5 in aprotic solvents were determined, revealing the formation of supramolecular oligomers. Compounds 1-5 generate organogels in chloroform or in acetone, leading in a second sol-gel transcription step to hybrid membrane materials on a nanoscopic scale. The crystal structures of 1-5 indicate that the arrangement is mainly defined by periodic parallel sheets, resulting from the alignment of hydrophobic organic and inorganic silica layers. Hybrid materials MB 1-MB 4, with a similar lamellar structure, define particularly attractive functional transport devices; they are oriented along the organic layers and sandwiched between the two siloxane layers. These systems have been employed successfully to design solid dense membranes and illustrate how the self-organised hybrid materials perform interesting and potentially useful functions.