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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]