Atomic-level structural editing is a promising way for facile synthesis and accurately constructing dielectric/magnetic synergistic attenuated hetero-units in electromagnetic wave absorbers (EWAs), but it is hard to realize. Herein, utilizing the rapid explosive volume expansion of the CoFe-bimetallic energetic metallic triazole framework (CoFe@E-MTF) during the heat treatment, the effective absorption bandwidth and the maximum absorption intensity of a series of atomic CoFe-inserted hierarchical porous carbon (CoFe@HPC) EWAs can be modified under the diverse synthetic temperature. Under the filler loading of 15 wt%, the fully covered X and Ku bands at 3 and 2.5mm for CoFe@HPC800 and the superb minimum reflection loss (RLmin )of -53.15dB and specific reflection loss (SRL) of -101.24dB mg-1 mm-1 for CoFe@HPC1000 areachieved. More importantly, the single-atomic chemical bonding among Co─Fe on the nanopores iscaptured by extended X-ray absorption fine structure, which reveals the formation mechanism of nanopore-confined vortical dipoles and magnetic domains. This work heralds the infinite possibilities of atomic editing EWA in the future.