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We studied a gradient anti-oxidation coating of C/C composite materials for aircraft brake discs with a simple process and low costs. The gradient coating consists of two layers, of which the inner layer is prepared with tetraethyl orthosilicate (Si (OC2H5)4), C₂H₅OH, H₃PO₄ and B₄C, and the outer layer is prepared with Na₂B₄O₇.10H₂O, B₂O₃, and SiO₂ powder. The experimental results show that after being oxidized at 700 °C for 15 h, the oxidation weight loss of the sample with the coating was only −0.17%. At the same time, after 50 thermal cycles in air at 900 °C, the sample’s oxidation weight loss was only −0.06%. We conducted the 1:1 dynamic simulation test for aircraft brake discs, and the brake disc did not oxidize, thus meeting the requirements for aircraft use. In addition, the anti-oxidation mechanism of the coating was analyzed via scanning electron microscopy (SEM), X-ray diffraction (XRD), differential thermal analysis (DSC-TGA), and high-temperature in situ SEM.