A series of wheat-gluten-based nanocomposites were produced by dispersing Cloisite-30B nanoclay particles into plasticized wheat gluten systems under thermal processing conditions. The exfoliation of the nanoparticles as confirmed by wide-angle X-ray diffraction and transmission electron microscopy has resulted in significant enhancement of the mechanical properties for both deamidated proteins and vital gluten systems under 50% relative humidity (RH). Such strength improvement was also pronounced for wheat gluten (WG) systems under a high humidity condition (RH = 85%). A similar level of further strength enhancement was obtained for the WG systems that had been strengthened by blending with poly(vinyl alcohol) (PVA) and cross-linking with glyoxal. Although the nanoclay modifier, a quaternary ammonium, caused an additional plasticization to the materials, the interactions between the gluten matrix and the nanoparticles were predominant in all of these nanocomposites. A solid-state NMR study indicated that the polymer matrix in all of these nanocomposites displayed a wide distribution of chain mobilities at a molecular level (less than 1 nm). The interactions between the nanoparticles and the natural polymer matrix resulted in motional restriction for all components in the mobile phases including lipid, plasticizers, and plasticized components, although no significant influence from the nanoparticles was obtained in the mobility of the rigid phases (unplasticized components). On a scale of 20-30 nm, the deamidated protein systems tended to be homogeneous. The small domain size of the matrix resulted in modifications of the spin-lattice relaxation of these systems via spin diffusion. The residual starch seemed to remain in a relatively larger domain size in WG systems. The nanoparticles could enhance the miscibility between the starch and the other components in the WG nanocomposite, but such miscibility enhancement did not occur in the WG/PVA blend and the cross-linked system. These polymer matrixes were still heterogeneous on a scale of 20-30 nm.