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.