Graphene oxide nanosheet (GO) is a multifunctional platform for binding with nanoparticles and stacking with two dimensional substrates. In this study, GO nanosheets were sonochemically decorated with zinc oxide nanoparticles (ZnO) and self-assembled into a hydrogel of GO–ZnO nanocomposite. The GO–ZnO hydrogel structure is a bioinspired approach for preserving graphene-based nanosheets from van der Waals stacking. X-ray diffraction analysis (XRD) showed that the sonochemical synthesis led to the formation of ZnO crystals on GO platforms. High water content (97.2%) of GO–ZnO hydrogel provided good property of ultrasonic dispersibility in water. Ultraviolet-visible spectroscopic analysis (UV–vis) revealed that optical band gap energy of ZnO nanoparticles (∼3.2 eV) GO–ZnO nanosheets (∼2.83 eV). Agar well diffusion tests presented effective antibacterial activities of GO–ZnO hydrogel against gram-negative bacteria (E. coli) and gram-positive bacteria (S. aureus). Especially, GO–ZnO hydrogel was directly used for brush painting on biodegradable polylactide (PLA) thin films. Graphene-based nanosheets with large surface area are key to van der Waals stacking and adhesion of GO–ZnO coating to the PLA substrate. The GO–ZnO/PLA films were characterized using photography, light transmittance spectroscopy, coating stability, scanning electron microscopy (SEM), energy-dispersive x-ray spectroscopic mapping (EDS), antibacterial test and mechanical tensile measurement. Specifically, GO–ZnO coating on PLA substrate exhibited stability in aqueous food simulants for packaging application. GO–ZnO coating inhibited the infectious growth of E. coli biofilm. GO–ZnO/PLA films had strong tensile strength and elastic modulus. As a result, the investigation of antibacterial GO–ZnO hydrogel and GO–ZnO coating on PLA film is fundamental for sustainable development of packaging and biomedical applications.
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