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Silk fibroin and three kinds of graphene-based materials (graphene, graphene oxide, and reduced graphene oxide) have been widely investigated in biomedical fields. Recently, the hybrid composites of silk fibroin and graphene-based materials have attracted much attention owing to their combined advantages, i.e., presenting outstanding biocompatibility, mechanical properties, and excellent electrical conductivity. However, maintaining bio-toxicity and biodegradability at a proper level remains a challenge for other applications. This report describes the first attempt to summarize the hybrid composites’ preparation methods, properties, and applications to the best of our knowledge. We strongly believe that this review will open new doors for coming researchers.