Atomic Infusion Induced Reconstruction Enhances Multifunctional Thermally Conductive Films for Robust Low‐Frequency Electromagnetic Absorption

@C (FWC-O@C) as the absorber and aramid nanofibers (ANFs) as the matrix was prepared. Driven by an atomic gradient infusion reduction strategy, the carbon atoms of absorbers can be precisely relocated from carbon shell to core oxometallate lattice, triggering in situ carbothermic reduction for customization of unique oxometallate-carbide heterojunctions and surface geometrical structure. Such an atoms reconstruction process effectively regulates interface electronic structure and magnetic configuration, resulting in enhanced polarization loss from abundant heterointerfaces and crystal defects and magnetic loss from hierarchical structure endowed magnetic coupling interaction, which jointly contributes to the efficient low-frequency EM absorption performance. Eventually, optimized FWC-O@C microplate exhibits a broad absorption bandwidth surpassed the entire C band, and the assembled FWC-O@C/ANFs composite film also performs a high thermal conductivity over 2500 % higher than that of the pure ANFs. These findings provide a new insight into the atomic reconstruction affected EM properties and a generalized methodological guidance for preparing multifunctional thermally conductive composite films.