Difficulty of multicomponent regulation and nanostructure design make it challenging to fabricate high-performance electromagnetic wave (EMW) absorption materials. Herein, pomegranate-like Fe3C@graphitic carbon embedded in amorphous carbon matrix (Fe3C@GC/AC) is successfully prepared through a viable heating induced self-assembly strategy. By adjusting carbonization temperature, controllable electromagnetic parameters and impedance matching characteristics of Fe3C@GC/AC nanocomposites could be acquired. Besides, dielectric loss and magnetic loss are offered by GC and Fe3C, while the amorphous carbon not only disperse Fe3C@GC nanoparticles well, but also strengthens interface polarization. The detailed analysis show that Fe3C@GC/AC nanocomposites exhibit excellent EMW absorption performance under the combined function of unique pomegranate-like nanostructure and various loss mechanisms of multi-components. Moreover, the strongest reflection loss value of optimal sample (RCF-700) is up to −96.3 dB (loss of EMW above 99.99999%) with a matching thickness of 2.08 mm, and the effective absorption bandwidth (EAB, RL < −10 dB) covers 6.38 GHz (11.62–18.0 GHz, covering Ku-band). In addition, the EAB can reach 14.08 GHz with the simulated thickness varies from 1.0 to 5.0 mm, covering 88% of the measured frequency range. The deep exploration of the bio-inspired structure of multi-component system provides a creative and effective way for high-performance EMW absorbers.
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