In this article, the silk fibroin (SF)/graphene oxide (GO)-blended nanofibers with one bioinspired nanostructure are fabricated via electrospinning. The morphology, chemical structure, antibacterial activity, and biocompatibility of the blending nanofibers are investigated. The results indicate that GO plays an important role in preparing the distinctive bioinspired structure. The antibacterial activity and in vivo cell culture test demonstrate that blending of GO could improve the antibacterial activity and biocompatibility of SF nanofibers. The blended nanofibers developed in this study may have considerable potential for wound dressing applications.