Large quantities of hazardous ceria-based polishing powder waste (CPPW) are produced worldwide each year, much of which unfortunately ends up in landfills, causing waste of rareearth resources and harm to the environment. This study proposes a novel mechanochemical approach for the recovery of La and Ce from CPPW and the regeneration of rare-earth polishing powders. The mechanochemical process facilitates the breakdown of the insoluble components of the CPPW (CeO 2 , CeLa 2 O 3 F 3 , LaF 3 ), enabling the leaching of 99.2% of La, 97.85% of Ce, and 98.53% of REOs. A comprehensive examination of the potential mechanochemical enhancement of rare-earth extraction mechanisms reveals that mechanochemistry can achieve the reduction of Ce(IV) to Ce(III) under non-high-temperature and high-pressure conditions, which can significantly enhance the leaching efficiency of Ce from CPPW. In order to ascertain the reason why the simultaneous leaching of La and Ce in the product could not be achieved, the leaching kinetics of La and Ce were simulated and discussed separately. After mechanochemical and acid leaching, the La,Ce-enriched leachate was separated and purified, for efficiently removing impurities (Si, Al, Na, Ca, Mg, Fe, etc.), and thus, 99.2 wt % purity of rare-earth polishing powder (CeO 2 and LaOF mixture) products were successfully regenerated. The chemical mechanical polishing results show that the as-regenerated rare-earth polishing powder exhibits excellent polishing performance and fulfils the requirements of commercial quality. This methodology presents a practicable solution for green, large-scale, efficient, and economical recovery of rare earths from the CPPW.