This study explores the phenomenon of molecular rolling lubrication in graphite nanosheets (GNSs) at cryogenic temperatures, which is a significant breakthrough in tribology. The research reveals that under cryogenic conditions (77 K), GNSs exhibit edge self-curling, leading to the formation of graphite nanorollers. This process results in ultra-low friction and wear rates, demonstrating the potential for molecular rolling lubrication. The study provides experimental evidence for this phenomenon, including parallel nanorollers observed at the friction interface. The molecular rolling lubrication mechanism is elucidated from an electronic interaction perspective, with the driving force being the uneven atomic shrinkage-induced stress. The shear force promotes the formation of intact nanorollers, while atomic vibration constraints reduce stress dissipation, favoring nanoroller formation. This work opens new avenues for controlling friction at the microscale and nanostructural manipulation, with potential applications in various fields such as sensing, optics, and tribology.This study explores the phenomenon of molecular rolling lubrication in graphite nanosheets (GNSs) at cryogenic temperatures, which is a significant breakthrough in tribology. The research reveals that under cryogenic conditions (77 K), GNSs exhibit edge self-curling, leading to the formation of graphite nanorollers. This process results in ultra-low friction and wear rates, demonstrating the potential for molecular rolling lubrication. The study provides experimental evidence for this phenomenon, including parallel nanorollers observed at the friction interface. The molecular rolling lubrication mechanism is elucidated from an electronic interaction perspective, with the driving force being the uneven atomic shrinkage-induced stress. The shear force promotes the formation of intact nanorollers, while atomic vibration constraints reduce stress dissipation, favoring nanoroller formation. This work opens new avenues for controlling friction at the microscale and nanostructural manipulation, with potential applications in various fields such as sensing, optics, and tribology.