This study investigates the regulatory mechanism of trace Fe on the electromagnetic wave (EMW) absorption properties of graphene-based materials. The authors propose a carrier injection strategy by designing Fe/reduced graphene oxide (RGO) heterogeneous interfacial materials to enhance the dielectric dispersion properties of graphene. The key findings include: 1. **Carrier Injection Strategy**: The Fe/RGO composite is synthesized through an electrostatic adsorption reaction and low-temperature thermal reduction method. The Fe nanosheets are uniformly dispersed on the RGO sheets, forming a face-to-face contact pattern to increase the contact area. 2. **EMW Absorption Performance**: The Fe/RGO-2 composite exhibits superior EMW absorption properties compared to pure RGO. It achieves a minimum reflection loss (RLmin) of −53.38 dB at 2.45 mm thickness and an effective absorption bandwidth (EAB) of 7.52 GHz (10.48–18 GHz) at a low filler loading of 2 wt%. 3. **Mechanism Analysis**: The enhanced EMW absorption is attributed to the carrier injection behavior from Fe to graphene at the interface, resulting in increased charge accumulation and rearrangement. This leads to increased interfacial and dipole polarization, as well as conductance loss. The off-axis electron hologram testing, simulation calculations, and carrier transport property experiments confirm these mechanisms. 4. **Conclusion**: The Fe/RGO composite demonstrates significant improvements in EMW absorption performance, providing a reliable strategy for the controllable fabrication of lightweight EMW absorbing materials. The study highlights the importance of understanding the dielectric polarization behavior of graphene-based materials and offers a new approach to designing high-performance EMW absorbing materials. This work was supported by various national and regional research funds, and the authors declare no conflict of interest.This study investigates the regulatory mechanism of trace Fe on the electromagnetic wave (EMW) absorption properties of graphene-based materials. The authors propose a carrier injection strategy by designing Fe/reduced graphene oxide (RGO) heterogeneous interfacial materials to enhance the dielectric dispersion properties of graphene. The key findings include: 1. **Carrier Injection Strategy**: The Fe/RGO composite is synthesized through an electrostatic adsorption reaction and low-temperature thermal reduction method. The Fe nanosheets are uniformly dispersed on the RGO sheets, forming a face-to-face contact pattern to increase the contact area. 2. **EMW Absorption Performance**: The Fe/RGO-2 composite exhibits superior EMW absorption properties compared to pure RGO. It achieves a minimum reflection loss (RLmin) of −53.38 dB at 2.45 mm thickness and an effective absorption bandwidth (EAB) of 7.52 GHz (10.48–18 GHz) at a low filler loading of 2 wt%. 3. **Mechanism Analysis**: The enhanced EMW absorption is attributed to the carrier injection behavior from Fe to graphene at the interface, resulting in increased charge accumulation and rearrangement. This leads to increased interfacial and dipole polarization, as well as conductance loss. The off-axis electron hologram testing, simulation calculations, and carrier transport property experiments confirm these mechanisms. 4. **Conclusion**: The Fe/RGO composite demonstrates significant improvements in EMW absorption performance, providing a reliable strategy for the controllable fabrication of lightweight EMW absorbing materials. The study highlights the importance of understanding the dielectric polarization behavior of graphene-based materials and offers a new approach to designing high-performance EMW absorbing materials. This work was supported by various national and regional research funds, and the authors declare no conflict of interest.