FeSiCr/CoFe2O4 composites were prepared by mechanical ball milling of cobalt ferrite prepared by hydrothermal method and flaky FeSiCr alloy powder. The phase and element of the composites was observed by XRD and XPS. The microstructure and surface elements of the composites were observed by SEM and EDS. The findings from the analyses confirmed the successful synthesis of the FeSiCr/CoFe2O4 composites. The results of EMP tests indicated that the electromagnetic parameters were balanced and the impedance matching was improved. When the mass percentage of cobalt ferrite was 20 %, the impedance matching was the best, and the RLmin reached −41.04 dB at 4.8 GHz. And the maximum EAB reached 5.4 GHz. By adjusting the thickness of the absorber, the EAB can be extended to 9.5 GHz (2.6–12.05 GHz), encompassing the entire C-band and X-band. The EMA performance of the composites has been greatly improved. FeSiCr/CoFe2O4 composites may serve as potential microwave absorbing materials in the future due to the wide range of economical raw materials, strong microwave absorption capacity and extensive absorption frequency range.