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Although strong and effective absorption of electromagnetic waves in the X-band region is of utmost importance for practical applications, it still faces many challenges. In this work, we prepared Fe2O3-decorated Ti3C2 composites via a facile one-step solvothermal route. Scanning electron microscopy micrographs showed that Fe2O3 particles effectively cover the Ti3C2 surface and insert into the Ti3C2 layers. X-ray diffraction patterns demonstrated that the Fe2O3 particles are beneficial for the Ti3C2 delamination. A high attenuation constant and suitable impedance matching enabled wide-range microwave absorption properties; however, the minimum reflection loss was relatively high. To achieve both wide bandwidth and strong absorption, we designed a multi-layered structural absorber. When the thickness was 1.9 mm, the fourfold-layered structural absorber exhibited the optimal absorption properties with the minimum RL value of − 49.68 dB at 9.922 GHz and RL less than − 10.82 dB in the entire X-band region. Therefore, the synthesized multi-layered structural Ti3C2/Fe2O3 composites can be used for practical applications as a high-performance microwave absorber in the X-band region. [ABSTRACT FROM AUTHOR]