To realize the application potential of molybdenum disulfide (MoS 2 ) in aqueous environments, scalable and efficient methods for the preparation of high-concentration and stable dispersions need to be developed. In this paper, ultrathin MoS 2 successfully was synthesized using an in situ-exfoliated bulk MoS 2 method in water using ionic liquid crystals (ILCs) as green exfoliating/dispersing agents. The ILCs containing hydrophobic cations and hydrophilic anions not only help to exfoliate bulk MoS 2 into ultrathin MoS 2 nanosheets but also prevent the reagglomeration of the ultrathin MoS 2 nanosheets in water. MoS 2 nanosheets were confined by the ILCs through π−π and C−H•••π interactions, preventing direct contact of MoS 2 with water. The ILC−MoS 2 dispersion exhibited remarkable dispersion stability exceeding 8 months at room temperature. Moreover, the ILC−MoS 2 dispersion has been successfully proven to be an excellent water-based lubricant, where the ILCs form a lubricant film on the friction surface through electrostatic interactions and MoS 2 increases the load-bearing capacity of the lubricant film due to its high modulus, resulting in an 84.9% reduction in the coefficient of friction compared to pure water. The method is expected to provide a new idea for the preparation and application of MoS 2 .