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As a promising microwave absorber filler, molybdenum disulfide (MoS 2 ), because of the unique structure, high electrical conductivity, and polarization effect, is receiving more and more interest. Developing MoS 2 -based composites with specific structure and morphology is a hot top in the field of microwave absorbers, because of its strong multiple scattering and reflecting for microwaves as well as its unique interfacial characteristics. Now, with a facile solvothermal method, a novel core−shell CoFe 2 O 4 @1T/2H-MoS 2 composite is synthesized, where the CoFe 2 O 4 nanospheres are entirely embedded in a special three-dimensional (3D) nest-like 1T/2H phase MoS 2 . Notably, in comparison with superparamagnetic CoFe 2 O 4 nanospheres, the coercivities of as-synthesized CoFe 2 O 4 @1T/2H-MoS 2 composites greatly increase. Here, 1T/2H-MoS 2 exhibits ferromagnetism superimposed onto large diamagnetism. It is noted that, by adjusting the content of 1T/2H-phase MoS 2 , the microwave absorption performance of as-synthesized composites can be effectively tuned. The combination of 1T/2H-MoS 2 with CoFe 2 O 4 helps to adjust the permittivity and optimize the impedance matching of the composites. Impressively, a minimum reflection loss (RL min ) of −68.5 dB for the as-synthesized composites with a thickness of 1.81 mm is gained at 13.2 GHz; meanwhile, a broad effective bandwidth of 4.56 GHz ranged from 13.2 to 17.76 GHz is achieved at 1.6 mm. Further, the overall effective bandwidth (RL < −10 dB) is obtained up to 14.5 GHz from 3.5 to 18.0 GHz, covering more than 90% of the measured frequency range. The high microwave absorption performance is ascribed to the special structure design with the core of magnetic CoFe 2 O 4 nanospheres and the shell of dielectric nest-like 1T/2H-MoS 2 as well as their appropriate impedance matching. From the perspective of basic research and practical microwave application, this study provides another feasible and effective pathway to design novel MoS 2 -based magnetic/dielectric microwave absorbers.

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