Flaky FeSiCr@Ni0.5Zn0.5Fe2O4 composites are successfully synthesized via ball milling and hydrothermal method. The microstructure, morphology, and phase composition of flaky FeSiCr@Ni0.5Zn0.5Fe2O4 composites are analyzed using X‐Ray diffractometer, energy dispersive spectroscopy, scanning electron microscope, and transmission electron microscope techniques. The electromagnetic wave absorption characteristics of the composite with varying contents of Ni0.5Zn0.5Fe2O4 are comprehensively investigated. The results show that the introduction of Ni0.5Zn0.5Fe2O4 reduces the permittivity, improves the synergistic effect of magnetic loss and dielectric loss, optimizes the impedance matching, and enhances the overall electromagnetic performance of the composites. The sample prepared with a composition of 40 wt% Ni0.5Zn0.5Fe2O4 displays the most pronounced absorption performance. The RLmin (reflection loss) reached −41.3 dB at 4.3 GHz, and the maximum effective absorption bandwidth (EAB) reaches 5.6 GHz which is 7–8 times that of the original sample. Notably, through adjusting the thickness of composites, the EAB could be broadened to 10.5 GHz (2.5–13.0 GHz), encompassing the entire C and X bands. The flaky FeSiCr@Ni0.5Zn0.5Fe2O4 composites have the advantages of wide source of raw materials, strong microwave absorption ability, and wide absorption frequency range, and are expected to become a potential microwave absorption material in the future.