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Polyethylene terephthalate (PET) and CO₂, two chemical wastes that urgently need to be transformed in the environment, are converted simultaneously in a one‐pot catalytic process through the synergistic coupling of three reactions: CO₂ hydrogenation, PET methanolysis and dimethyl terephthalate (DMT) hydrogenation. More interestingly, the chemical equilibria of both reactions were shifted forward due to a revealed dual‐promotion effect, leading to significantly enhanced PET depolymerization. The overall methanol yield from CO₂ hydrogenation exceeded the original thermodynamic equilibrium limit since the methanol was in situ consumed in the PET methanolysis. The degradation of PET by a stoichiometric ratio of methanol was significantly enhanced because the primary product, DMT was hydrogenated to dimethyl cyclohexanedicarboxylate (DMCD) or p‐xylene (PX). This synergistic catalytic process …