Achieving precise control over the magnetic properties of composite materials for specific applications, while simultaneously optimizing their magnetic, dielectric, and electrical characteristics, remains a formidable challenge in material science. This study addresses this challenge by systematically modulating the magnetic and electrical properties of ZrO2/Fe3O4-Fe/C nanocomposites through controlled variations in the Zr/Fe ratio and leveraging electron transfer-induced effects. First-principles calculations reveal that reducing the Zr/Fe ratio decreases ZrO2 content, thereby limiting the transfer of unpaired electrons to ZrO2. This limitation leads to the accumulation of localized electrons, significantly enhancing the magnetic moments from 136.29 to 165.76 mu B. The fine-tuning of the Zr/Fe ratio enables precise electron transfer control, unlocking synergistic optimization of magnetic, dielectric, and electrical properties. Notably, the 4-ZrO2/Fe3O4-Fe/C-700 composite demonstrated exceptional electromagnetic wave absorption performance, achieving a minimum reflection loss (RLmin) of-67.76 dB and an effective absorption bandwidth (EAB) of 6.11 GHz with a thickness of only 2.4 mm. These results not only highlight breakthrough in tailoring magnetic properties via electron transfer but also advance the understanding of the intricate interplay between magnetic regulation mechanisms and functional properties. This study provides a robust foundation the development of next-generation magnetic materials with multifunctional applications, which has great application potential in the field of stealth technology.