Controllable Design of “Nested Doll” MoS₂/V₂O₃ Heterostructures Promotes Polarization Effects for High‐Efficiency Microwave Absorption

Abstract Special multilayer heterostructures and lattice modulation play a crucial role in the field of microwave absorption. Herein, a unique “nested doll” MoS₂/V₂O₃ heterostructures are synthesized via crystal epitaxy growth and solvothermal strategy. The synchronized modulation of lattice spacing and interfacial vacancies in MoS₂ nanosheets is achieved by adjusting the S²⁻ concentration. A high concentration of S²⁻ expands the MoS₂ lattice spacing and increases interfacial vacancies, facilitating the precise modulation of the orderly arrangement of MoS₂‐V₂O₃‐MoS₂ layers and inducing interfacial polarization. By increasing the number of V₂O₃‐MoS₂ layers from two to five, a built‐in electric field is formed, which enhances charge transfer from the MoS₂ surface to the V₂O₃ core. The introduction of vacancies reduces the MoS₂ band gap, lowers the electron hopping barrier, increases dielectric loss, and ultimately synergistically improves microwave absorption (MA). As a result, the “nested doll” MoS₂/V₂O₃‐5 (5 layers) microspheres exhibit superior MA behavior compared to other MoS₂/V₂O₃ absorbers. The reflection loss reaches −69.65 dB and the effective absorption bandwidth achieves 7.68 GHz. These discoveries have contributed to the further development of multilayer heterostructures and improved advances in the theory of energy band structures and electromagnetic properties.