Self-dispersed graphene crumpled balls (GCBs) demonstrate exceptional tribological performance as lubricant additives at elevated temperatures. However, the critical relationships among unique wrinkle architectures, internal porosity characteristics, and resultant dispersion stability/friction-reduction mechanism remain insufficiently explored. In particular, the synergistic effects arising from structural hierarchy and surface chemistry modulation in high-temperature lubrication systems require systematic investigation. Herein, we propose a wrinkle engineering strategy guided by Stokes’ law to fabricate surface modifier-free GCBs with programmable three-dimensional geometries. Systematic investigations reveal that the degree of crumpling on the GCBs critically dominates the dispersion characteristics and the interlayer shearing resistance. When molybdenum disulfide quantum dots (MoS₂ QDs) are deposited on GCBs, a more consistent and robust tribochemical reaction film can form on the friction interface in response to severe damage. Compared with commercial high-temperature chain oil (CH-27Q), this complex achieves an over 2-fold increase in anti-friction efficiency. Overall, this study establishes a structure–performance paradigm for developing autonomous lubrication systems under extreme thermal conditions.

Inorganic nanoparticles have been proved as powerful lubricant additives at elevated temperature. However, the tribological properties are inevitably impaired due to poor dispersion and insufficient high temperature resistance of organic matter modified nanoparticles. Here, we prepare a self-dispersed molybdenum disulfide quantum dot/graphene crumpled ball (MGCB) comprising molybdenum disulfide quantum dot uniformly interspersed on the wrinkled graphene ball. The crumpled ball composite possesses excellent dispersity in polyalkylene glycol base oil without depending on surface modifiers. Compared with the conventional phosphate esters lubricant, our results indicate MGCB could vastly improve the lubrication performance of polyalkylene glycol with an extremely low concentration (0.05 wt%) at elevated temperature (150 °C), showing a friction reduction of 47% and a wear reduction of 30% compared with the conventional phosphate esters lubricant (tricresyl phosphate, TCP). This is because crumpled ball potentiates synergistic lubrication effect within the boundary lubrication. Overall, we envision our designed self-dispersed MGCB has significant potential in tribological application at elevated temperature.