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Considering the poor mechanical properties of regenerated collagen materials, the possibility of creating stronger and tougher collagen composite materials attracts particular research interests. In this study, we report that GO (Graphene oxide)-multiwalled carbon nanotube (MWNT) nanomaterials were constructed by using GO dispersed MWNT, and the strength and toughness of collagen fibers were significantly improved by introducing GO-MWNT nanomaterials into the collagen matrix during dry-jet wet spinning that exhibits the advantage of positive stretching to the extruded fiber before coagulation. We found that the combination of GO and MWNT can enhance the dispersion of both in the collagen matrix. Due to their strong interactions, they can not only spontaneously form the GO-MWNT network but also mutually induce collagen molecules to self-assemble and form aligned fibrils microstructure in dry-jet wet spinning process and resulting hybrid fibers. The interconnected networks of orderly aligned GO and MWNT can greatly enhance the interfacial interactions by forming hydrogen bonds with collagen molecules, resulting in the synergistic enhancement of the tensile strength, toughness and thermal stability of collagen hybrid fibers. This study provided asimple and environmentally friendly pathway to generate collagen-based fiber materials with improved performances and could be suitable for amyriad of biomedical applications.

Novel collagen/GO-MWNT hybrid fibers with improved strength and toughness by dry-jet wet spinning