The interlayer coupling interaction of bentonite (BT) material behave superior performance and unique functionality by introducing guest functional molecules. As intercalation agents, ionic liquids (ILs) with high polarity and molecular structure regulation can provide excellent lubricity and multifunctionality. Herein, the novel IL-modified intercalation bentonite (IL-BT) were designed and prepared by functionalization of the imidazolium-based and phosphorus-based ILs. And ultra-thin lamellar structure morphology is obtained, which contributes to the enhanced dispersion and stability in base oils. For IL -BT, their strong interlayer slip can significantly improve lubrication properties. Besides, FIB-TEM results show that unique tribofilm is detected at the sliding asperity. The excellent tribological properties are attributed to the synergistic lubricity of interlayer slip, tribo-chemical reaction and repair effect during friction.