AbstractRecently, the design and development of efficient microwave absorbents by facile engineering approaches have attracted much attention. Particularly, some unique structures caused by cross‐scale design are promising in enhancing the absorbing capability toward microwave irradiation. Herein, the cross‐scale design strategy is implemented to enhance the electromagnetic wave absorption performance of polymetallic sulfides (PMS). In PMS, the dipole polarization unit is optimized, and the distribution of electronic states is improved by doping Ti atoms; Meanwhile, the MS/M3S4 homogeneous hetero‐phases interfaces is constructed in PMS using a phase separation strategy; and the conductivity of PMS is modulated by the addition of acetylene black (ACET). The cross‐scale synergy of microwave absorption leads to a significant enhancement of the microwave absorption (MA) performance of PMS/ACET composites. The optimal reflection loss value of Ti‐LES with 10% ACET addition reaches −55.49 dB and the effective absorption bandwidth reaches 6.73 GHz. The 17.5% ACET‐conditioned Ti‐HES achieves a reflection loss of −37.2 dB at a low frequency of 4.8 GHz. This study not only provides a novel strategy for the development of new broadband MA materials but also validates a new idea for the multi‐scale synergistic optimization of MA materials.
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