The rational design and exploration of the metal oxide-carbon composite are greatly desired for enhanced supercapacitor application. Herein, we develop a novel Bi2MoO6 and carbon sphere hybrid material as a supercapacitor electrode via a simple solvothermal process. The microstructural analysis of the carbon sphere@Bi2MoO6 reveals that the 10 nm thick Bi2MoO6 nanopetals are consistently anchored on the carbon spheres surface, forming a 3-dimensional nanoarchitecture. The carbon sphere@Bi2MoO6 electrode displays an excellent specific capacitance of 521.42 F g-1 at 1 A g-1, which is one of the best values of any reported Bi2MoO6-based electrodes to date. Moreover, this hybrid electrode can accumulate total charge as high as 2083 C g-1, which is consistent with high capacitance. The all-solid-state symmetric supercapacitor device exhibited the specific capacitance of 26.69 F g-1, along with â-80% of capacitance retention after 10000 cycles. The superior supercapacitor performance of the carbon sphere@Bi2MoO6 electrode is primarily due to the hierarchical nanoarchitecture of Bi2MoO6, its promotion of redox reactions, and the presence of highly conductive carbon spheres at cores, which provides pathways for rapid electron transfer. These results highlight feasibility of the carbon sphere@Bi2MoO6 hybrid material as a highly propitious electrode for supercapacitor applications.