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Materials with a high saturation magnetization have gained increasing attention in the field of microwave absorption; therefore, the magnetization value depends on the magnetic configuration inside them. However, the broad-band absorption in the range of microwave frequency (2-18 GHz) is a great challenge. Herein, the three-dimensional (3D) Fe/C hollow microspheres are constructed by iron nanocrystals permeating inside carbon matrix with a saturation magnetization of 340 emu/g, which is 1.55 times as that of bulk Fe, unexpectedly. Electron tomography, electron holography, and Lorentz transmission electron microscopy imaging provide the powerful testimony about Fe/C interpenetration and multi-domain state constructed by vortex and stripe domains. Benefiting from the unique chemical and magnetic microstructures, the microwave minimum absorption is as strong as −55 dB and the bandwidth (<−10 dB) spans 12.5 GHz ranging from 5.5 to 18 GHz. Morphology and distribution of magnetic nano-domains can be facilely regulated by a controllable reduction sintering under H2/Ar gas and an optimized temperature over 450–850 °C. The findings might shed new light on the synthesis strategies of the materials with the broad-band frequency and understanding the association between multi-domain coupling and microwave absorption performance

Broadening microwave absorption via a multi-domain structure