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Summary: The rational strategy to design the well‐ordered morphology of the metal oxides with defective engineering and tailoring them into specific electrode fabrication can significantly improve their electrochemical properties for high‐performance energy storage systems. Herein, we adopted an effective strategy to introduce oxygen‐defect into the well‐ordered three‐dimensional flower‐like CoMoO4 nanoarchitecture. The Co‐Mo precursor leads to the introduction of oxygen‐defects into the CoMoO4 (rCMO) nanoarchitecture during the heat‐treatment under an oxygen‐controlled environment (argon). The oxygen‐defects in the material could facilitate abundant electroactive sites and intrinsically enhance the conductivity and supercapacitor performance. The oxygen‐defect CoMoO4 (rCMO) exhibits a specific capacity of 531 mAh g−1 at a current density of 1 A g−1 compared to the pristine CoMoO4 (CMO; ambient atmosphere) of 322 mAh g−1 under the same current density. Meanwhile, the fabricated hybrid supercapacitor (HSC) of rCMO//AC provides a maximum specific capacitance of 159 F g−1. Further, it distributes an energy density of 49.87 Wh kg−1 at the power density of 845.45 W kg−1 with an excellent cyclic life of ~91.03% over 10 000 cycles. [ABSTRACT FROM AUTHOR]