Designable electromagnetic parameters accompanied by a low density of metal–organic framework (MOF)-derived metal/carbon composites are essential prerequisites for excellent microwave-absorbing materials. However, the conventional route is confined to slight modification of the physicochemical properties of metal species and carbon, which also restricts the functionalization of MOF-derived materials. Here, a facile technique has been improved by making full use of highly porous structure to uniformly introduce metallic Co nanoparticles into carbon matrix derived from Cu3(btc)2. Through changing the starting amount of Co sources, the composition of the final products can be tuned, offering an effective route to control electromagnetic properties. Multiple attenuation mechanisms are employed to realize excellent reflection loss performance, which can be clarified by modified equivalent circuit mode. Effective frequency bandwidth (fe) over the whole X band can be obtained by optimizing interfacial polarizati...