Inorganic nanomaterials exhibit superior friction-reduction and anti-wear properties in oils. In this study, 2D layered α-zirconium phosphate (α-ZrP) nanosheets intercalated with different amines have been synthesized to study their dispersion stabilities in lubricating oil and tribological applications. The intercalated amines should be sufficiently long and lipophilic to provide stabilization to α-ZrP nanosheets in mineral oil. The results of tribological tests illustrate that with the addition of well-dispersed nanosheets, the coefficient of friction (COF) and pin volume loss reduce by ~47% and 75%, respectively. The excellent dispersion stability enables the nanosheets to flow into the contact area at the beginning, and thereby protect the rubbing surface. A reduction in the van der Waals forces between the adjacent layers induced by the intercalated amines transforms the friction between adjacent layers from pin disk to sliding, leading to a decrease in the COF under hydrodynamic lubrication. The study provides a new method to enhance the tribological properties via tuning the dispersion stabilities of nanomaterials in oils.