| Summary: | Abstract This work reports the fabrication of a large‐sized hydrogel sheet with enhanced mechanical and adhesive properties. The fabrication involves the introduction of carboxymethyl‐modified cellulose nanofibers (m‐CNFs) and solid silica nanoparticles (SSNs) as physical cross‐linkers into acrylic acid monomer (AA), followed by bar coating and photopolymerization. The addition of the nanomaterials to the monomer solution renders it viscous, enabling the fabrication of A4‐sized hydrogel sheets with uniform thickness and enhanced mechanical and adhesive properties. Interestingly, the combined incorporation of both the nanomaterials generates a synergistic effect to improve the properties much more, which results from the hierarchical rupture of the multiple hydrogen‐bonded interactions among the poly(acrylic acid) (PAA) matrix, m‐CNFs, and SSNs. Under optimal conditions, the hydrogel sheet incorporated with the dual crosslinkers exhibits a sevenfold higher toughness and a sixfold increased peel strength than plain PAA, together with good biocompatibility. Furthermore, when mesoporous silica nanoparticles (MSNs) with active agent loading into their pores are incorporated instead of SSNs, the active agent can be released from the hydrogel sheet in a sustained or temperature‐sensitive manner, indicating that the system is potentially applicable to transdermal drug delivery system with no additional adhesive.
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