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In order to improve the high‐temperature friction and wear properties of polyimide (PI), Mo2CTx/PI nanocomposite materials are prepared by using 2D Mo2CTx MXene as reinforcement. Compared with the properties of pure PI, Mo2CTx/PI nanocomposites exhibit significant improvement on thermal stability, hardness, and tribological performance. Especially, the addition of Mo2CTx can reduce friction coefficient and wear rate of PI significantly at different temperatures ranging from room temperature (RT) to 200 °C. The hardness and the thermo‐degradation temperature of composites increase due to the formation of an organic inorganic structure. In addition, this structure helps to form a protective film containing Mo2CTx nanoflakes, iron oxide, molybdenum oxide, and organic compounds during friction, and improve the tribological properties of PI composite.
2D Mo2CTx nanomaterials are uniformly dispersed in polyimide matrix by a simple hot‐pressing method as reinforcement. The friction coefficient and wear rate of composites are significantly improved at elevated temperatures, which is contributed by the formation of protective and transfer film containing 2D Mo2CTx nanoflakes, iron oxide, molybdenum oxide, and organic compounds during friction.