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The N‐(4‐hydroxyphenyl) maleimide (4‐HPM) modified waterborne polyurethane emulsions (MWPU) were used as surface sizing agents to improve the interfacial adhesion between carbon fibers (CF) and epoxy resin matrix. Dynamic light scattering (DLS), transmission electron microscope (TEM), and thermogravimetric analysis (TGA) showed the particle size distribution, storage stability, and thermal stability of the modified MWPU. And the surface reactivity of CF increased significantly after sizing. The interfacial shear strength (IFSS) and the interlaminar shear strength (ILSS) of CFREs were tested, and the fracture morphology was observed. The result showed that a continuous and uniform sizing layer is formed on the surface of CF. In particular, the comprehensive performance and interfacial modification effect of the MWPU emulsion outperformed other samples when the 4‐HPM content was 1.0 wt%. Compared with unsized carbon fibers, the IFSS and ILSS are up to 71.30% and 30.81% higher, respectively.

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To improve the interfacial bonding effect of carbon fibers (CFs) and epoxy resins, we prepared a fluorine‐containing high‐epoxy‐value sizing agent (named TS) in this article. It is an emulsion with a more uniform particle size distribution and higher stability better than a commercial Takemoto sizing agent. In addition, sulfonic acid groups can improve the hydrophilicity of the TS, and the presence of epoxy groups enhances the wettability between CFs and the matrix. The properties of the sizing agents were examined by Fourier transform infrared spectroscopy, dynamic light scattering, and thermogravimetric analysis. The sized CFs were evaluated by scanning electron microscopy, x‐ray photoelectron spectroscopy, monofilament tensile test, and dynamic contact angle. Afterward, CF/epoxy composites were prepared, and their fracture morphology and interlaminar shear strength (ILSS) were examined. Results indicated that the TS sizing significantly increased the content of activated carbon on the surface of the CFs and improved the bonding effect between the fiber and the matrix. After TS was sized, the ILSS increased from 49.64 to 58.74 MPa, 18.34% higher than unsized CF/epoxy composites, showing the prominent interfacial reinforcement better than commercial Takemoto.