Although the chemical recycling of polymers synthesized by controlled radical polymerization enables the recovery of pristine monomer at low temperatures, it operates efficiently under strictly anaerobic conditions. Instead, oxygen-tolerant depolymerizations are scarce, and are either restricted to the use of a boiling co-solvent or are performed in closed vessels, often suffering from low conversions. Here, an open-vessel, oxygen-tolerant depolymerization of atom transfer radical polymerization (ATRP)-synthesized polymers is introduced, leading to high percentages of monomer regeneration (>
90% depolymerization efficiency). Dissolved oxygen is eliminated by either utilizing high catalyst loadings, or lower catalyst loadings combined with a radical initiator. Notably, the methodology is compatible with various solvents (i.e., anisole, 1,2,4-trichlorobenzene (TCB), 1,2-dichlorobenzene (DCB), etc.) and a range of commercially available ligands including tris 2-(dimethylamino)ethylamine (Me