Fractal Topology Directed 3D Conductive Metal–Organic Frameworks: Coordination Mode Regulation and Multiscale Electromagnetic Wave Absorption Mechanisms

Abstract Conductive metal–organic frameworks (cMOFs) enable precise optimization of electromagnetic wave (EMW) absorption performance through structural design and composition regulation. However, periodic networks with linear or planar structures are constrained by their dimensional characteristics and exhibit single EMW scattering paths alongside insufficient energy dissipation efficiency. This study proposes a method combining DFT‐driven structural design with solution phase assembly, and a series of 3D cMOFs that exhibit ordered conductivity, together with spin polarization characteristics, are successfully constructed. Fe‐THQ‐1, Fe‐THQ‐2, and Fe‐HHB featuring 3D architectures and hierarchical pores are strengthened of the dielectric loss leveraging the continuous conductive network; meanwhile, ordered coordination triggered magnetic anisotropy coupled with electron spin. Synergistically, it concomitantly enhanced electromagnetic (EM) loss, providing multi‐scale scattering paths plus efficient polarization centers for EMW. Compared with planar structures, the 3D architectures achieved an effective absorption bandwidth (EAB)with a five orders of magnitude boost, and the reflection loss (RL) demonstrated an improvement of ≈1000%. Benefiting from the tunability of spatial topological patterns, the 3D cMOFs further enabled dynamic migration of EMW absorption bands spanning Ku to X. The novel strategy involving stereoscopic coordination for synergistic enhancement of EM loss may provide insights into constructing multi‐dimensional loss synergy and frequency‐tunable EMW absorption materials.