Superlubricity of graphite sliding against graphene can be easily attained at the nanoscale when it forms the incommensurate contact under a low contact pressure. However, the achievement of superlubricity under an ultrahigh contact pressure (>1 GPa), which has more applications in the lubrication of micromachine and nanomachine, remains unclear. Here, this problem is addressed and the robust superlubricity of graphite is obtained under ultrahigh contact pressures of up to 2.52 GPa, by the formation of transferred graphene nanoflakes on a silicon tip. The friction coefficient becomes as low as 0.0003, a state that is attributed to the extremely low shear strength of the graphene/graphite interface in the incommensurate contact. When the pressure exceeds some threshold, the superlubricity state collapses suddenly with the friction coefficient increasing ≈10 times. The failure of superlubricity originates from the delamination of the topmost graphene layers on graphite under ultrahigh contact pressures, which requires the tip to provide additional exfoliation energies during the sliding process. The results demonstrate that the superlubricity of graphite sliding against graphene can exist stably under ultrahigh contact pressure, which would appear to accelerate its application in nanoscale lubrication.

2D or 3D layered materials, such as graphene, graphite, and molybdenum disulfide, usually exhibit superlubricity properties when sliding occurs between the incommensurate interface lattices. This study reports the superlubricity between graphite and silica under ambient conditions, induced by the formation of multiple transferred graphene nanoflakes on the asperities of silica surfaces after the initial frictional sliding. The friction coefficient can be reduced to as low as 0.0003 with excellent robustness and is independent of the surface roughness, sliding velocities, and rotation angles. The superlubricity mechanism can be attributed to the extremely weak interaction and easy sliding between the transferred graphene nanoflakes and graphite in their incommensurate contact. This finding has important implications for developing approaches to achieve superlubricity of layered materials at the nanoscale by tribointeractions.