Maintaining the electrochemical activity of cobalt-based oxide electrodes is crucial for ion storage, yet rationally regulating their activity remains a significant challenge. This study develops a Bacillus cereus “biomineralization” strategy to construct a composite electrode material consisting of hollow-derived carbon rods (LY) coated with oxygen vacancy-rich Co3O4-x nanosheets (LY-Co3O4-x). The hollow LY provides a 3D conductive network, prevents nanosheet aggregation, and shortens ion diffusion paths.The highly dispersed Co3O4-x nanosheets rich in oxygen vacancies boost the pseudocapacitive effect, improving the electrochemical activity of Co3O4. The interfacial coupling within LY-Co3O4-x promotes electron redistribution and facilitates rapid charge transfer, accelerating the processes of Pb2+ hydration, dehydration of the hydration shell, and ion desolvation. Leveraging these advantages, LY-Co3O4-x exhibits outstanding Pb2+ removal performance. When used as a cathode, it achieves a Pb2+ adsorption capacity of 78.7 mg g−1 and an adsorption rate of 2.62 mg g−1 min−1, at 1.60 V, with excellent stability. This discovery opens a new pathway for utilizing microbial redox reactions to construct metal oxides and regulate their electrochemical activity.