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Continuous carbon fiber reinforced polymer composite 3D printing has drawn more attention due to its ability to manufacture composite structures with complex shapes. The surface treatment of CF is necessary to improve the combination between carbon fiber (CF) and matrix. In this work, polyurethane with nano‐SiO2 (PU/SiO2) was used to size CF to enhance the compatibility of CF and nylon 6 (PA6). The chemistry and morphology of the CF were characterized by Fourier transform infrared spectroscopy (FTIR), X‐ray photoelectron spectroscopy (XPS), and scanning electron microscopy (SEM). The interface strength between CF and PA6 was tested by the fiber pull‐out test, and eventually obtained optimized concertation of PU/SiO2 sizing agents (with 25 wt% PU and 0.4 wt% nano‐SiO2). The results show that compared with untreated CF, the interfacial shear strength (IFSS) of CF and PA6 after sizing increased by 316.93%. In addition, several CF/PA6 composite specimens printed by a homemade composite 3D printer were used to do mechanical tests. The results show that the flexural strength increased by 33.87%, the tensile strength increased by 20.75%, and the interlaminar shear strength (ILSS) increased by 66.54%. [ABSTRACT FROM AUTHOR]