Carbon-based microwave absorbing composites with magnetic-dielectric properties and multiple loss mechanism are considered to be an effective choice for solving electromagnetic pollution. In this paper, the PPy/Fe/Fe3O4@C composite was synthesized from MIL-101-Fe derivatives and subsequently coated polypyrrole (PPy) by combining hydrothermal, high-temperature pyrolysis and oxidative polymerization. The effects of pyrolysis temperature and PPy loading on components, microstructures and electromagnetic parameters were investigated. The results showed that the PPy/Fe/Fe3O4@C composite consisted of two-dimensional carbon flakes modified by magnetic particles and laminated conductive polymers. When the PPy loading is moderate, the composite reaches a minimum reflection loss (RLmin) of −61.38 dB at a 3.1 mm thickness and effective absorption bandwidth (EAB) of 5.81 GHz at the thickness of 2.2 mm. After pyrolysis, the unique three-dimensional structure of carbon sheet stacking, as well as the heterogeneous interface and conductive networks generated by the modification of magnetic particles Fe and Fe3O4 and conductive PPy, are beneficial to improve the dielectric and magnetic losses to optimize the impedance matching. These conductive polymer-modified magnetic-dielectric composites have potential for development and application in microwave absorption.
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