The application of Fe-based amorphous microspheres in high-performance electromagnetic wave absorbing materials is significantly limited by a single loss mechanism. Utilizing interfacial engineering and magnetic-dielectric synergistic effect is a viable approach to enhance microwave absorption. In this work, FeSiBCuNbZr amorphous microspheres were synthesized using single copper roller melt-spinning method and ball mill method. The finding reveals that the incorporation of SiO2 and TiO2(B) (bronze phase TiO2) shells notably enhances polarization loss and conductive loss. FeSiBCuNbZr@SiO2@TiO2(B) amorphous composites exhibited a minimum reflection loss value of −64.89 dB at a thickness of 2.17 mm and an effective absorption bandwidth (EAB) of 8.08 GHz covering 9–18 GHz at a thickness of 1.9 mm. The exceptional wave absorption performance is ascribed to the combined effect of magnetic loss in the FeSiBCuNbZr amorphous core and dielectric loss from the double-shell structure, while maintaining favorable impedance matching. This work provides a new core–shell FeSiBCuNbZr amorphous composites for efficient electromagnetic wave absorption.
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