Over the past decade, there have been many interesting studies in the scientific literature about the interaction of graphene-based polymeric nanocomposites with microorganisms to tackle antimicrobial resistance. These studies have reported variable intensities of biocompatibility and selectivity for the nanocomposites toward a specific strain, but it is widely believed that graphene nanocomposites have antibacterial, antiviral, and antifungal activities. Such antibacterial activity is due to several mechanisms by which graphene nanocomposites can act on cells including stimulating oxidative stress; disrupting membranes due to sharp edges; greatly changing core structure mechanical strength and coarseness. However, the underlying mechanisms of graphene nanocomposites as antiviral and antifungal agents remain relatively scarce. In this review, recent advances in the synthesis, functional tailoring, and antibacterial, antiviral, and antifungal applications of graphene nanocomposites are summarized. The synthesis of graphene materials and graphene-based polymeric nanocomposites with techniques such as pressurized gyration, electrospinning, chemical vapor deposition, and layer-by-layer self-assembly is first introduced. Then, the antimicrobial mechanisms of graphene membranes are presented and demonstrated typical in vitro and in vivo studies on the use of graphene nanocomposites for antibacterial, antiviral, and antifungal applications. Finally, the review describes the biosafety, current limitations, and potential of antimicrobial graphene-based nanocomposites.