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Plastic imposes a critical threat to the environment, ecosystems and human health, because of low utilization efficiency of plastics. Here, we demonstrate a sustainable highly efficient cascade photocatalysis for upcycle plastics to value-added acetic acid using Fe single atom catalysts (Fe@C3N4 SAC) at ambient conditions. Inspired by Phanerochaete chrysosporium microbial, the defected Fe@C3N4 SAC acts as a as a bifunctional cascade photocatalyst for both Fenton-like and CO2 reduction reactions. During the reaction, hydroxyl radicals (*OH) form and subsequently oxidize plastics into CO2 intermediates. These CO2 intermediates were then photo-reduced to CH3COOH on the same catalyst via cascade photocatalysis. The mechanismmore » was confirmed by in situ multimodal microscopy and spectroscopies, with density functional theory calculations. A state-of-art CH3COOH yield of 63.8 mg h-1 gcat-1 from PVC, 12.7 mg h-1 gcat-1 from PE, 5.4 mg h-1 gcat-1 from PET, and 5.3 mg h-1 gcat-1 from PP were directly obtained under AM1.5G solar irradiation and further validated under real sunlight (~ 0.6 sun), achieving 5.6 mg h-1 gcat-1 from PET, using low-cost Fe@C3N4 SAC in a sealed reactor by enhancing the photon transport and utilization efficiency. The techno-economic analysis shows it is promising to practically mitigate plastic based on broader social welfare assessments.« less