Two-dimensional metal carbide or nitride materials are considered as a new class of electromagnetic wave absorbing materials due to their unique multilayer structure and metal-like properties. The NiSe2-CoSe2@C/Ti3C2Tx composites were prepared through a facile hydrothermal treatment and selenization reaction. Distinctly, the maximum reflection loss (RL) is −60.46 dB with the mass fraction of NiSe2-CoSe2@C/Ti3C2Tx of 40 wt% at 2.6 mm. The bandwidth of RL < −10 dB reaches up to 5.68 GHz (10.32–16 GHz). The synergistic mechanism of the multiple scattering and multi-interface polarization effects of NiSe2-CoSe2@C compounded with Ti3C2Tx is reviewed to interpret the significant improvement of electromagnetic wave absorption performance. The results indicate that NiSe2-CoSe2@C/Ti3C2Tx composites have potential applications as realistic electromagnetic wave absorbing materials.