Friction as a fundamental physical phenomenon dominates nature and human civilization, among which the achievement of molecular rolling lubrication is desired to bring another breakthrough, like the macroscale design of wheel. Herein, an edge self-curling nanodeformation phenomenon of graphite nanosheets (GNSs) at cryogenic temperature is found, which is then used to promote the formation of graphite nanorollers in friction process towards molecular rolling lubrication. The observation of parallel nanorollers at the friction interface give the experimental evidence for the occurrence of molecular rolling lubrication, and the graphite exhibits abnormal lubrication performance in vacuum with ultra-low friction and wear at macroscale. The molecular rolling lubrication mechanism is elucidated from the electronic interaction perspective. Experiments and theoretical simulations indicate that the driving force of the self-curling is the uneven atomic shrinkage induced stress, and then the shear force promotes the intact nanoroller formation, while the constraint of atomic vibration decreases the dissipation of driving stress and favors the nanoroller formation therein. It will open up a new pathway for controlling friction at microscale and nanostructural manipulation.

Graphite lubrication is not effective in vacuum, and the failure mechanism is still under debate. Here, we show that graphene as two-dimensional (2D) “graphite paper” can overcome this shortcoming of graphite. Graphene exhibits stable super-low friction in a vacuum environment at the engineering scale because it can self-form a highly ordered lamellar structure on the sliding interface during the friction process owing to its unique 2D nano-effects. Experimental observation of the layer-slip phenomenon on the low-energy-state outside layers provides direct evidence to understand the lubrication mechanism of graphitic materials.