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Supercapacitors have been extensively studied due to their advantages of fast-charging and discharging, high-power density, long-cycling life, low cost, etc. Exploring novel nanomaterial schemes for high-performance electrode materials is of great significance. Herein, a strategy to combine vertical graphene (VG) with MoO₃ nanosheets to form a composite VG/MoO₃ nanostructure is proposed. VGs as transition layers supply rich active sites for the growth of MoO₃ nanosheets with increasing specific surface areas. The VG transition layer further improves the electric contact and adhesion of the MoO₃ electrode, simultaneously stabilizing its volume and crystal structure during repeated redox reactions. Thus, the prepared VG/MoO₃ nanosheets have been demonstrated to exhibit excellent electrochemical properties, such as high reversible capacitance, better cycling performance, and high-rate capability.