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Highlights Hierarchical Fe3O4-Fe@CNFs/Al-Fe3O4-Fe nanocomposites were constructed by in situ growth, vacuum-assisted filtration, and self-reduction methods. The carbon framework, with in situ grown magnetic nanoparticles, supports two-dimensional magnetic nanosheets, achieving excellent electromagnetic performance and good impedance matching. Excellent reflection loss value (− 59.3 dB), broadband wave absorption (5.6 GHz at 2.2 mm thickness), and low radar cross-section value were achieved.