Abstract: Designing integrated strategies to optimize the impedance matching and electromagnetic (EM) loss capability of FeSiCr has become a key factor in expanding its application in field of EM absorption. The integration of four strategies, namely magnetic-dielectric composite, flaky morphology, laminated structure and magnetic/magnetic heterointerfaces is considered a feasible solution. Herein, laminated FeSiCr composites were prepared by embedding ~ 8 nm carbonyl iron nanoparticles in FeSiCr flakes followed by phosphating treatment. The composite has magnetic-dielectric dual loss, enhanced magnetic loss, multiple reflection, reduced permittivity, and enhanced permeability to optimize impedance matching and EM loss ability for efficient EM absorbing performances. Compared with raw composites, laminated carbonyl iron/FeSiCr@FePO4 composites reach the minimal reflection loss of -54.73 dB, an increase of 83%, and effective absorption bandwidth (EAB) of 6.96 GHz, an increase of 17.6%, which are endowed by the special microstructure. Furthermore, EAB can be effectively extended to 12.89 GHz at only 5.0 mm thickness through gradient structure design, and radar cross reduction value also can exceed 10 dB·m2 at 10.9-15.2 GHz. This work not only deepens the understanding of magnetic/magnetic heterointerfaces, but also enhances the loss capability and expands EAB, thus contributing to EM absorption applications.