The intercalation of long-chain primary amines into the laminar matrices of MoS2 or V2O5-gel leads to well ordered, lamellar organic-inorganic nanocomposites. Powder X-ray diffraction analysis, stoichiometry determined by chemical analysis, and considerations on the molecular volume of the guest and surface available indicate the guest is oriented in the interlaminar space with their molecular axis perpendicular to the matrix plane. The hydrothermal treatment of these products leads to the formation of multiwall nonotubes with the organic component intercalated between inorganic layers. The composition and the shape of the tubes indicate that the tube formation should occur by the rolling up of precursor laminae.