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Novel polyimide/fluorinated graphene oxide (PI/FGO) nanocomposites with outstanding mechanical, thermal, and tribological properties were obtained using FGO nanosheets which were successfully fabricated by simple hydrothermal reaction. FGO exhibited distinguished interface adhesion with PI matrix due to covalent bonds, resulting improved mechanical and wear resistance of PI/FGO nanocomposites. Wherein, PI/FGO‐0.5 nanocomposite demonstrated conspicuous tribological performance accompanied with 33.1% decrease of friction coefficient and 80.8% reduction of wear rate compared with pure PI under dry friction. Notably, PI/FGO nanocomposites manifested better wear resistance under seawater than that under dry friction, illustrating its great potentiality as high wear‐resistant material suitable for ocean environment.

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