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A novel composite containing CoSe and porous carbon polyhedra (PCP), denoted as CoSe@PCP, was successfully synthesized using Co-based zeolitic imidazolate framework (ZIF-67) as precursor through a two-step method, including carbonization of ZIF-67 and subsequent selenization. The field-emission scanning electron microscopy and transmission electron microscopy characterizations confirm that CoSe nanoparticles are uniformly dispersed in PCP. When the CoSe@PCP was used as anode material for lithium-ion batteries, it exhibits superior performance with a high reversible capacity of 675 mAh g⁻¹ at 200 mA g⁻¹ after 100 cycles and 708.2 mAh g⁻¹ at 1 A g⁻¹ after 500 cycles as well as excellent cycling stability. Additionally, the CoSe@PCP also demonstrates excellent performance as anode material for sodium-ion batteries. A reversible capacity of 341 mAh g⁻¹ can be obtained over 100 cycles at …