The eco-friendly menthol-modified carbon dots (CDs-Menth) were synthesized for the first time and exhibited the particularly promising application potential as additives of polyalphaolefin (PAO4). On the one hand, the CDs-Menth could be well dispersed into PAO4 with excellent and long-term dispersion stability via a convenient and green mean, that is, the solvation effect of petroleum ether. This mean was far more advanced to current strategies such as chemical modifications and adding dispersants. On the other hand, the CDs-Menth as additives possessed not only the duty-bound merits such as the distinguished friction-reducing, anti-wear, and load-carrying functions, but also an amazing ability of self-repairing effect. The repairing rate of lower disc in the ball-on-disc friction pair lubricated with CDs-Menth/PAO4 lubricant (2.5 wt %) was about 19.3% if the friction duration was prolonged from 20 to 120 min. Meanwhile, the wear volume reduction for PAO4 caused by CDs-Menth remarkably increased from 43.5 to 74.6%. By virtue of the self-repairing effect, the CDs-Menth could form the tough and tensile boundary lubrication films on the rubbing surfaces, not only tremendously reducing the friction and wear of friction pair, but also hopefully protecting the friction interfaces from the potential oxidation and corrosion.