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Nowadays, it is quite difficult to develop a facile, efficient, and easy large-scale production method to obtain the composite that can maintain a balance of Electromagnetic interference (EMI) shielding properties and mechanical properties. Herein, this work adopted the technology of electrohydrodynamic atomization deposition (EHDAD), layer-by-layer (LbL) assembly and heat-pressing to prepare carbon fiber fabric/graphene oxide/Fe 3 O 4 /epoxy (CFf/GO/Fe 3 O 4 /epoxy) composite. The research results show that the CFf/GO/Fe 3 O 4 /epoxy composite can maintain a good balance between mechanical and EMI performance. More specifically, the tensile strength of CFf/GO/Fe 3 O 4 /epoxy-4 composite can reach 565.1 MPa, which is higher than that of other composites reported previously. This can be attributed to the synergistic effect of covalent bonds and van der Waals forces improved the mechanical properties of the composite. Benefitting from the unique multi-layer structure and the synergistic effect of nanoparticles, the EMI shielding performance of CFf/GO/Fe 3 O 4 /epoxy composite can reach a maximum of 32.9 dB. The improvement of the EMI properties of composite was mainly attributed to the dielectric loss and magnetic loss. Surprisingly, the composite has excellent mechanical stability and EMI shielding stability even after long periods of storage. It is believed that this work opens up more possibilities to provide EMI shielding materials with outstanding mechanical properties. [Display omitted] • The facile, efficient and easy large-scale production method was adopted to fabricate carbon fiber fabric/graphene oxide/Fe 3 O 4 /epoxy composites. • The EMI shielding effectiveness of the multilayer-structured composite can achieve 32.9 dB, which can meet commercial applications. • The mechanical property of the composite was improved to 565.1 MPa owing to the synergistic effect of covalent bond and van der Waals force. [ABSTRACT FROM AUTHOR]