Electroactive cobalt oxide (Co3O4) exhibits great promise as an anode material for lithium-ion batteries (LiBs) owing to its high theoretical capacity. However, its potential application faces challenges posed by low conductivity and poor cycling stability. In this study, a comprehensive multi-strategic approach was employed to fabricate a high-performance Co3O4-based anode. The approach involved utilizing Co–Cu bimetallic metal-organic frameworks (MOFs) anchored on a stainless-steel mesh (SSM) as the precursor. The resulting free-standing anode comprises Cu-doped porous Co3O4 nanosheets, offering several advantageous characteristics such as being binder-free, possessing a hierarchically porous architecture, and demonstrating improved conductivity and structure stability. This combination of merits results in a material that exhibits significantly enhanced electrochemical performance, featuring high specific capacity, excellent cycling stability, and remarkable rate performance. This multi-strategic exploration of metal oxides with tailored surface area and pore size enables the precise design and fabrication of advanced anodes, specifically optimized for the demanding requirements of LiBs.