The weak fiber-matrix interface is a bottleneck hindering the development of carbon fiber composites. In this work, an optimized electrophoretic deposition (EPD) approach was explored to improve the interfacial properties by depositing uniformly two-dimensional MXene (Ti3C2Tx) nanoparticles onto the surface of carbon fibers (CF). The MXene-CF hybrids were then used to fabricate continuous carbon fiber reinforced polymer (CFRP) composites. The results manifested that the presence of MXene nanoparticles on the CF surfaces could significantly increase the fiber surface energy and wettability, as well as their surface roughness. As a result, a remarkable increase of the interfacial strength and flexural properties of CFRP has been observed. The functionalized MXene–CF–epoxy composites witnessed a prominent enhancement of interlaminar shear strength (ILSS), flexural strength and monofilament tensile strength compared to their unfunctionalized counterparts. The versatile EPD strategy proposed herein, constitutes a promising approach for CFRP modification that can lead to significantly improved performance.