It is a great challenge to utilize graphene for practical applications in moving parts, which meet high contact pressure and atmosphere environments. In this work, ultralow friction (0.054) of graphene was achieved under high contact pressure (1.03 GPa) and atmosphere environment via the operando formation of PbS quantum dots (QDs)/graphene heterojunction at the frictional interface. It is found that PbS QDs are trapped in graphene nanosheets via shear-induced rearrangement for obtaining the PbS QDs/graphene heterojunctions, which provide an excellent rolling effect to lower friction. It is also found that the heterogeneous PbS QDs/graphene tribofilms have a strong Pb-enriched function and heterojunction nanorod phase. Our objective is to uncover the physical and chemical mechanisms governing the friction of 0D/1D nanostructures within PbS QDs/graphene heterostructures through our studies. This research will enhance our comprehension of nanomaterials' frictional behavior while offering valuable guidance and optimization strategies for their application in mechanical engineering and functional nanomaterials. Consequently, our efforts aim to foster the advancement of nanoscience and technology, leading to additional scientific and technological breakthroughs.