Supramolecular self-assemblies based on multiple noncovalent forces have emerged as an effective way to fabricate multistimuli-responsive and self-healable intelligent materials. However, the development of supramolecular nanostructures as advanced functional materials in practical fields is always subjected to their relatively weaker mechanical strength and overuse of organic components. In this work, we proposed a new strategy to construct self-supported supra molecular hydrogels with the features of tunable mechanical strength, high water content, and self-healing properties through the hierarchically organic inorganic hybridization of Laponite matrix with cyclodextrin-based pseudopolyrotaxanes. Notably, the mechanical properties of the obtained hydrogels can be conveniently modulated by tuning the molecular weight of polymeric chains in the central pseudopolyrotaxanes, which may provide a feasible way to promote the practical application of supramolecular metamaterials in miscellaneous fields.