T.T. Nguyen, Junji Nakamura, Kaveh Edalati
ABSTRACT Global CO 2 emissions and plastic pollutants are two of the most urgent environmental challenges. Here, we report a unified photocatalytic strategy that simultaneously converts CO 2 and polyethylene terephthalate (PET) waste into value‐added products under light irradiation. CO 2 is selectively reduced to CO with over 95% selectivity, while PET is transformed to methane, terephthalate, ethylene glycol, glycolate, and acetate. This dual process is enabled by a distorted high‐entropy oxide (BaTiNbTaZnO 9 ), containing electron‐accepting d 0 cations (Ba, Ti, Nb, and Ta), electron‐donating d 1 0 cations (Zn), and Lewis‐basic Ba sites for CO 2 adsorption, whose distorted atomic environment was confirmed by synchrotron X‐ray adsorption spectroscopy. The cooperative use of CO 2 and plastic as complementary redox partners eliminates sacrificial agents and enhances redox efficiency compared with conventional CO 2 conversion. Beyond mitigating two persistent pollutants, this solar‐driven approach also suggests a pathway for microplastic degradation, establishing a scalable concept for integrated waste‐to‐fuel technologies.