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Carbon fibrous (CF) membranes were fabricated by electrospinning, thermal stabilization, and the carbonization process. The in-depth analyses of the CF membranes' composition, structure, and microwave absorption (MA) property demonstrate that the MA performance of the membranes is strongly correlated with the C/O ratio and CF framework's microstructure. A maximum absorption value of −23.4 dB is achieved at 800 °C, and this was synergistically enhanced to −42.5 dB with the addition of graphene nanosheets (GNSs). The special multilayered membranes containing dielectric loss CNSs and CFs making the balance between excellent impedance matching and the high loss characteristic could deliver an excellent MA property. With the facile and controllable synthesis of the GNS/CF membranes, a new approach to efficiently optimize and regulate its MA behavior is now possible. [ABSTRACT FROM AUTHOR]