A novel and excellent composite film was fabricated by simply casting cassava silk fibroin (CSF), chitosan quaternary ammonium salt (HACC), and graphene oxide (GO) in an aqueous solution. Scanning electron microscope images showed that when GO was dispersed in the composite films, the surface of CSF-based composite film became rough, and a wrinkled GO structure could be found. When the content of GO was 0.8%, the film displayed a higher change with respect to the breaking strength and elongation, respectively, up to 97.69 ± 3.69 and 79.11 ± 1.48 MPa, keeping good thermal properties because of the incorporation of GO and HACC. Furthermore, the novel CSF/HACC/GO composite film demonstrates a lower degradation rate, implying the improvement of the resistance to the enzyme solution. Especially in the film with 0.8 wt% GO, the residual mass arrived at 64.35 ± 1.1% of the primary mass after 21 days compared with the CSF/HACC film. This would reclaim the application of silk-based composite films in the biomaterial field.
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