Controllable production of graphene by simultaneously exfoliating and reducing graphite oxide (GO) under dielectric barrier discharge (DBD) plasma with various working gases, including H₂ (reducing), Ar (inert) and CO₂ (oxidizing), has been investigated. The deoxygenation level of GO is related to the type of working gases while regardless of the bulk temperature during plasma discharge, which implicates a high-energy electron/ion bombardment deoxygenation mechanism. Acting as electrode materials in a supercapacitor cell with KOH electrolyte, graphene nanosheets (GS) from various plasmas exhibit high specific capacitance and good electrochemical stability. With the assistance of low temperature plasma, this approach has the potential to enable the fabrication of a broad spectrum of graphene-based composites that are sensitive to high temperatures.