To improve Li storage capacity and the structural stability of Ti₃C₂ MXene-based electrode materials for lithium-ion batteries (LIBs), a facile strategy is developed to construct three-dimensional (3D) hierarchical porous Ti₃C₂/bimetal-organic framework (NiCo-MOF) nanoarchitectures as anodes for high-performance LIBs. 2D Ti₃C₂ nanosheets are coupled with NiCo-MOF nanoflakes induced by hydrogen bonds to form 3D Ti₃C₂/NiCo-MOF composite films through vacuum-assisted filtration technology. The morphology and electrochemical properties of Ti₃C₂/NiCo-MOF are influenced by the mass ratio of MOF to Ti₃C₂. Owing to the interconnected porous structures with a high specific surface area, rapid charge transfer process, and Li⁺ diffusion rate, the Ti₃C₂/NiCo-MOF-0.4 electrode delivers a high reversible capacity of 402 mAh g⁻¹ at 0.1 A g⁻¹ after 300 cycles; excellent rate performance (256 mAh g⁻¹ at 1 A g⁻¹); and long-term stability with a capacity retention of 85.7% even after 400 cycles at a high current density, much higher than pristine Ti₃C₂ MXene. The results highlight that Ti₃C₂/NiCo-MOF have great potential in the development of high-performance energy storage devices.