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The fabrication of nanometer‐sized magnetic heterostructures with controlled magnetic components and specific interfaces holds great significance in the field of electromagnetic (EM) wave absorption. However, the process of achieving these structures still poses significant challenges. Here, abundant magnetic heterostructures are successfully fabricated by utilizing the surface energy anisotropy differences of the nonasymmetric hammer‐shaped interface to support the nucleation and growth of magnetic heterostructure components while effectively inhibiting their aggregation. Through a confined growth strategy via in situ growth of FeOOH and sequentially precise thermal treatments, dispersion of the heterostructures is achieved at the nanometer scale, while also observing a high degree of chemical stability due to occurrence of a charge‐compensation effect at the interface. Consequently, a series of magnetic heterostructures are obtained via phase translations of FeOOH precursors. The nanometer‐sized heterostructures demonstrate multilevel interfacial polarization effects. Furthermore, the hierarchical core–shell structure of the heterostructures promotes anisotropic polarization absorption. As a result, the multiple interfaces and nanometer‐sized Fe/Fe3O4@SiO2@Fe‐2 heterostructures demonstrate improved EM wave attenuation performance. Remarkably, they achieve an absorption bandwidth of 9 GHz at a thickness of 1.8 mm. A novel avenue is introduced here for investigating the intricate relationship between structure and properties in magnetic heterostructures. [ABSTRACT FROM AUTHOR]

Highlights: A novel FeCoNi carbon fiber (FeCoNi/CF) is obtained through an improved electrospinning technology, which greatly endows the fiber with strong magnetic property. The FeCoNi/CF exhibits an enhanced electromagnetic loss capability due to the construction of one-dimensional magnetic FeCoNi alloy. The designed one-dimensional FeCoNi/CF exhibits excellent performance, with a broad effective absorption band of 1.3 GHz in the low-frequency electromagnetic field at an ultrathin thickness of 2 mm, which provides a great potential for practical application in the future. Rational designing of one-dimensional (1D) magnetic alloy to facilitate electromagnetic (EM) wave attenuation capability in low-frequency (2–6 GHz) microwave absorption field is highly desired but remains a significant challenge. In this study, a composite EM wave absorber made of a FeCoNi medium-entropy alloy embedded in a 1D carbon matrix framework is rationally designed through an improved electrospinning method. The 1D-shaped FeCoNi alloy embedded composite demonstrates the high-density and continuous magnetic network using off-axis electronic holography technique, indicating the excellent magnetic loss ability under an external EM field. Then, the in-depth analysis shows that many factors, including 1D anisotropy and intrinsic physical features of the magnetic medium-entropy alloy, primarily contribute to the enhanced EM wave absorption performance. Therefore, the fabricated EM wave absorber shows an increasing effective absorption band of 1.3 GHz in the low-frequency electromagnetic field at an ultrathin thickness of 2 mm. Thus, this study opens up a new method for the design and preparation of high-performance 1D magnetic EM absorbers. [ABSTRACT FROM AUTHOR]