Solid inorganic lubricants are thermally stable but they are often limited by their lack of deformability, while organic lubricants have limitations in terms of thermal stability. In this study, a novel solid organic–inorganic nanocomposite lubricant that synergistically combines the thermochemically stable structure of a layered oxide with the relative softness of an organic polymer is presented. The nanocomposite is made by intercalating 11-aminoundecanoic acid in a lepidocrocite-type protonated titanate, H1.07Ti1.73O4. The amino acid molecules rapidly arrange to form a paraffinic bilayer in the gallery region of the layered host. This topotactic reaction yields a well-organized layered nanocomposite consisting of inorganic 2D titanate layers separated by amino acid molecules. Above elevated temperatures, 11-undecanoic acid polymerizes into nylon-11 confined between crystalline titanate monolayers. The lubricating properties of these nanocomposites up to 580 °C are determined using high-temperature pin-on-disc experiments using steel-steel contacts. The lubricative properties are based on the softening of the intercalated polymer above 200 °C. The encapsulation of the polymer chains by the inorganic titanate monolayers protects the organic component from thermal degradation and increases the thermal stability of the system.