Anion Doping as a “Trigger” to Modulate Defect‐Tailored Dielectric Coupling for Ultrathin Microwave Absorber

Abstract Anion doping engineering is recognized as a prospective strategy to adjust the electronic configuration and transport capacity of carbon‐based magnetoelectric hybrids and to optimize defects for the modulation of electromagnetic (EM) properties. This study effectively accomplishes an overwhelming enhancement in the dielectric coupling between conduction and polarization for the CuCo bimetallic/carbon system by employing in situ (N, O)/ex situ (S, Se) doping and defect modulation strategies. The well‐designed lattice distortions are facilitated by the large atomic radii (Se) intercalated carbon skeleton and the bimetallic CuCo, which activate the reinforcement of the dipole polarization in the high‐frequency region. Interestingly, an appropriate number of vacancies acts as “electron traps” to accelerate the local charge redistribution, endowing the system with extremely strong electronic interactions and interface‐induced polarization. It is remarkable that the ultra‐thin feature (1.8 mm) is able to achieve an extraordinary microwave attenuation (‒56.1 dB). Additionally, specific defect upgrading of anionic Se doping beneficially hinders the development of phonon transmission, conferring Cu 2 Se/CoSe 2 /NC‐Se aerogel outstanding infrared stealth capabilities along with inheriting the advantages of traditional carbon‐based hybrids (lightness, compressive/structural stability, and hydrophobicity/anti‐corrosive properties). This research offers distinctive perspectives on the advanced design of multifunctional absorbers in complex environments.