The arrival of the 5G era has made electromagnetic pollution a problem that needs to be addressed, and flexible carbon-based materials have become a good choice. In this study, wet continuous papermaking technology was used to prepare carbon fiber paper (CFP) with a three-dimensional conductive skeleton network; Molybdenum disulfide ( MOS2)/ iron (Fe) @ carbon fiber paper-based shielding material was prepared by impregnating and blending molybdenum disulfide/iron ( MOS2/Fe) phenolic resin MOS2/ Fe@ CFP. The morphology, structure, electrical conductivity, mechanical properties, hydrophobicity, and electromagnetic shielding properties of the composite were characterized. The results show that the three-dimensional network structure based on a short carbon fiber paper-based conductive skeleton and the synergistic effect of the MOS2 dielectric wave absorbing agent and Fe magnetic wave absorbing agent have good electromagnetic shielding performance. Conduct electromagnetic shielding simulation using HFSS software to provide options for the structural design of CFP. The electromagnetic shielding performance of CFP reaches 70 dB, and the tensile strength reaches 34.39 MPa. Based on the mechanical properties, the compactness of carbon fiber paper is ensured. The lightning damage model test using CST software expands the direction for the use of carbon fiber paper. In summary, MOS2/ Fe @CFP with excellent shielding performance has great application prospects in thinner and lighter shielding materials, as well as high sensitivity, defense and military equipment.