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To reach high energy density and excellent cycle stability, an asymmetric supercapacitor device combining a high-power electric double-layer capacitor (EDLC) anode and high energy density battery-type cathode has been designed and fabricated. A binder-free strategy was used to prepare cathode by coating graphene (G) on Ni foam (Ni), then electrodepositing MnO₂, followed by calcination process. The potentiodynamic (PD) electrodeposition cycles of MnO₂ onto graphene significantly impact the electrochemical properties. Benefiting from the hierarchical structure and binder-free process of the designed 75 C/G/Ni hybrid cathode, potentiostatic (PS) electrodeposition followed by PD electrodeposition for 75 cycles demonstrates a high specific capacitance of 691 F g⁻¹ at 2 A g⁻¹. The enhanced capacitive performance can be attributed to the synergistic effect between MnO₂ nanosheets and graphene, in which graphene can serve as ideal support matrix and conductive channels. Furthermore, an asymmetric supercapacitor was fabricated with 75 C/G/Ni and (G + AC)/Ni as the cathode and anode, respectively, and a carboxymethyl cellulose–potassium hydroxide (CMC-KOH) gel electrolyte. The 75 C/G/Ni//(G + AC)/Ni asymmetric supercapacitor (ASC) exhibits a maximum energy density of 43 kW kg⁻¹ at a power density of 302 W kg⁻¹ with a potential window of 1.6 V and maintains good cycling stability of 88% capacitance retention at 2 A g⁻¹ (over 5000 cycles). Four solid-state asymmetric supercapacitors stack connected in series display an effective 5.0 V working potential to increase the voltage and output energy as a device. The device was charged using a 18,650 Li battery with a voltage of +3.8 V for 30 s and discharged six white LEDs for 20 min. The facile fabrication and remarkable capacitive performance of the MnO₂/G/Ni hybrid make it a promising electrode candidate in electrochemical energy conversion/storage devices.