It is a challenge to design Ti3C2Tx MXene-based electromagnetic interference (EMI) shielding composites with excellent mechanical properties. Herein, a highly robust, flexible and durable Ti3C2Tx MXene/carbon fiber fabric/thermoplastic polyurethanes (Ti3C2Tx MXene/CFf/TPU) composite was fabricated through simple electrohydrodynamic atomization deposition, layer-by-layer stacking and hot pressing technology. The synergistic strengthening effect of van der Waals forces and covalent bonds can improve the tensile strength of the composite up to170.2 MPa, which is far greater than that of other MXene-based composites previously reported. In addition, the EMI shielding performance of the Ti3C2Tx MXene/CFf/TPU composite also improved with increasing MXene mass fraction, reaching 40.4 dB, which can be attributed to the dielectric loss provided by conductive fillers and the enhanced absorption within the sandwich structure. More interestingly, the composite retained excellent resistance stability, EMI-SE stability and flexibility, even after multiple bending and releasing cycles. This work provides a facile and environmentally-friendly method for preparing composites with excellent EMI shielding properties and mechanical properties, which may provide more possibilities for applications in intelligent wear and electronic wireless communication equipment.