Environment-friendly and sustainable deep eutectic solvents (DESs) are considered as a new type of lubricant. Here, MoSx/rGO nanohybrids were prepared as lubricant additive to improve the tribological performance of DES. The nanohybrids exhibited excellent dispersibility in DES. Tribological tests indicated that the DES with 1.5 wt% of MoSx/rGO additive exhibited the best lubrication performance for steel tribopair by reducing friction (∼31.2%) and wear (∼88.2%) due to the synergistic effect between the MoSx/rGO nanohybrid and DES. The superior lubricating properties of DES containing nanohybrids are primarily due to the attachment of nanohybrids to the friction interface, which triggers the formation of a robust tribofilm. These findings provide new insights into enhancing the tribological performance of DES by incorporating effective additives.