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Electromagnetic performance regulation in mid‐infrared (MIR) and microwave (MW) spectrums is crucially significant, which can be achieved by heterophase introduction and structural manufacturing. In this work, Si‐O amorphous phase is introduced into Pt film by magnetron co‐sputtering technique, the film thickness is optimized by adjusting deposition time. After annealing treatment, a double‐layered structure is constructed with the migration and growth of Pt crystals, in which the lower layer is composed of Pt coarse grains while the upper layer is Si‐O amorphous phase with embedded Pt fine grains. Furthermore, due to the thickness difference, diverse kinds of structural patterns (arrays or mesh) can be obtained with the solid‐state dewetting of the lower layer. According to the increasing thickness, the infrared emissivity can decrease from 0.67 to 0.25 (8–14 μm), demonstrating a great decline of apparent temperature of 162.9 °C when the background is 300 °C. And the microwave transmissivity also exhibits tremendous variation over 90% (from 96% to 5%), realizing the transformation from transmitting to shielding. [ABSTRACT FROM AUTHOR]

Nano‐heterointerface engineering has been demonstrated to influence interfacial polarization by expanding the interface surface area and constructing a built‐in electric field (BEF), thus regulating electromagnetic (EM) wave absorption. However, the dielectric‐responsive mechanism of the BEF needs further exploration to enhance the comprehensive understanding of interfacial polarization, particularly in terms of quantifying and optimizing the BEF strength. Herein, a “1D expanded 2D structure” carbon matrix is designed, and semiconductor ZnIn2S4 (ZIS) is introduced to construct a carbon/ZIS heterostructure. The cross‐dimensional nano‐heterointerface design increases interface coupling sites by expanding the interface surface area and induces an increase in the Fermi level difference on both sides of the interface to modulate the distribution of interface charges, thereby strengthening the BEF at the interface. The synergistic effect leads to excellent EM absorption performance (minimum reflection coefficient RCmin = −67.4 dB, effective absorption bandwidth EAB = 6.0 GHz) of carbon/ZIS heterostructure. This work introduces a general modification model for enhancing interfacial polarization and inspires the development of new strategies for EM functional materials with unique electronic behaviors through heterointerface engineering. [ABSTRACT FROM AUTHOR]