Nanocomposites with enhanced mechanical properties and efficient self-healing characteristics can change how the artificially engineered materials' life cycle is perceived. Improved adhesion of nanomaterials with the host matrix can drastically improve the structural properties and confer the material with repeatable bonding/debonding capabilities. In this work, exfoliated 2H-WS nanosheets are modified using an organic thiol to impart hydrogen bonding sites on the otherwise inert nanosheets by surface functionalization. These modified nanosheets are incorporated within the PVA hydrogel matrix and analyzed for their contribution to the composite's intrinsic self-healing and mechanical strength. The resulting hydrogel forms a highly flexible macrostructure with an impressive enhancement in mechanical properties and a very high autonomous healing efficiency of 89.92%. Interesting changes in the surface properties after functionalization show that such modification is highly suitable for water-based polymeric systems. Probing into the healing mechanism using advanced spectroscopic techniques reveals the formation of a stable cyclic structure on the surface of nanosheets, mainly responsible for the improved healing response. This work opens an avenue toward the development of self-healing nanocomposites where chemically inert nanoparticles participate in the healing network rather than just mechanically reinforcing the matrix by slender adhesion.
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