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The “block‐on‐plate” nanocomposite structure material is realized with the zeolitic imidazolate framework (ZIF‐67) on graphene oxide (GO) with surface oxygen‐rich functional groups. Scanning electron microscopy, X‐ray photoelectron spectroscopy, X‐ray diffractograms, fourier transform infrared spectroscopy, and ZIF‐67/GO demonstrate a high capability of promoting the lubricating performance of [Choline][Proline] ([CH][P]) bio‐ionic liquid. Specifically, the wear volume of the disc by [CH][P]‐0.1 ZIF‐67/GO is only 52% of the one lubricated by pure [CH][P]. Moreover, ZIF‐67/GO shows a long time, high dispersion stability in [CH][P]. In addition, the combination of GO nanosheets and ZIF‐67 can make ZIF‐67/GO have better polishing effect between the steels during the friction process, which can effectively form a robust lubrication layer and improves overall lubricating properties. As a result, the interfacial lubrication can be significantly improved by these newly developed [CH][P]‐ZIF‐67/GO lubricants. This work offers a new promising application for ZIF‐67 nanocomposites with GO in advanced lubrication systems. This work also provides a new strategy of producing lubricants containing nanoparticles with high dispersion stability, which may solve the biggest challenge in this field.

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