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Macroscale superlubricity on engineering steel surfaces offers a promising solution for minimizing friction and wear in engineering applications. However, achieving superlubricity typically requires a long running‐in period, which may result in significant wear for the friction pair. Herein, a new lubricant with superlubricating properties is rationally designed by using polyethylene glycol (PEG) and critic acid (CA) under complexing effect with a running‐in period of about 800 s. Importantly, the introduction of carbon quantum dots (CQDs) obtained from the pyrolysis of CA into PEG aqueous solution shortens the running‐in period for achieving macroscale superlubricity (µ ≈ 0.005) between steel/steel contact to 44 s. The corresponding wear rate (1.15 × 10−7 mm3 N−1 m−1) on the steel disk is reduced by 77% due to the shorter running‐in time. Furthermore, the surface analysis combined with the molecular dynamics simulations demonstrates that CQDs easily adsorb on the surface of the friction pair, forming a carbon film that reduces interaction energy between the lubricant molecules and the substrate. This work provides new insights into the lubrication mechanism of CQDs and contributes to the design of liquid superlubricants with short running‐in periods and low wear rates on engineering steel surfaces. [ABSTRACT FROM AUTHOR]