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
supramolecular 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.