Developing microwave absorption (MA) materials with ultrahigh efficiency and facile preparation method remains a challenge. Herein, a superior 1D@2D@1D hierarchical structure integrated with multi‐heterointerfaces via self‐assembly and an autocatalytic pyrolysis is designed to fully unlock the microwave attenuation potential of materials, realizing ultra‐efficient MA performance. By precisely regulating the morphology of the metal organic framework precursor toward improved impedance matching and intelligently integrating multi‐heterointerfaces to boosted dielectric polarization, the specific return loss value of composites can be effectively tuned and optimized to −1002 dB at a very thin thickness of 1.8 mm. These encouraging achievements shed fresh insights into the precise design of ultra‐efficient MA materials.
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