Layered palygorskite (PAL), commonly called attapulgite, is a natural inorganic clay mineral composed of magnesium silicate. In this study, an aqueous miscible organic solvent treatment method is adopted to prepare molybdenum-dotted palygorskite (Amo-PMo) nanoplatelets, which greatly improved the specific surface area of PAL and the dispersion effect in an oil-based lubricant system. Their layered structure and size were confirmed using transmission electron microscopy (TEM) and atomic force microscopy. Following a tribological test lubricated with three additives (PAL, organic molybdenum (SN-Mo), and Amo-PMo), it was found that the sample of 0.5 wt% Amo-PMo exhibited the best tribological properties with a coefficient of friction of 0.09. Moreover, the resulting wear scar diameter and wear volume of the sliding ball surface were 63% and 49.6% of those lubricated with base oil, respectively. Its excellent lubricating performance and self-repairing ability were mainly attributed to the generated MoS₂ adsorbed on the contact surfaces during the tribochemical reaction, thereby effectively preventing the direct collision between asperities on sliding solid surfaces. Thus, as-prepared Amo-PMo nanoplatelets show great potential as oil-based lubricant additives, and this study enriches the existing application of PAL in industry.