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The rational design of magnetic carbon composites, encompassing both their composition and microstructure, holds significant potential for achieving exceptional electromagnetic wave-absorbing materials (EAMs). In this study, FeCo@CM composites were efficiently fabricated through an advanced microwave plasma-assisted reduction chemical vapor deposition (MPARCVD) technique, offering high efficiency, low cost, and energy-saving benefits. By depositing graphitized carbon microspheres, the dielectric properties were significantly enhanced, resulting in improved electromagnetic wave absorption performances through optimized impedance matching and a synergistic effect with magnetic loss. A systematic investigation revealed that the laminar-stacked structure of FeCo exhibited superior properties compared to its spherical counterpart, supplying a higher number of exposed edges and enhanced catalytic activity, which facilitated the deposition of uniform and low-defect graphitized carbon microspheres. Consequently, the dielectric loss performance of the FeCo@CM composites was dramatically improved due to increased electrical conductivity and the formation of abundant heterogeneous interfaces. At a 40 wt% filling amount and a frequency of 7.84 GHz, the FeCo@CM composites achieved a minimum reflection loss value of −58.2 dB with an effective absorption bandwidth (fE) of 5.13 GHz. This study presents an effective strategy for developing high-performance EAMs.