Reductive Photocatalysis Unlocks the Hydrodeoxygenation of Polycarbonate Plastic Into Fuel‐Range Hydrocarbons

ABSTRACT Polycarbonate (PC) is among the most challenging plastics to recycle because its robust aromatic C─O linkages resist conventional depolymerization strategies. Here, we report the first visible‐light‐driven photocatalytic system for the reductive depolymerization and hydrodeoxygenation of PC under ambient conditions, selectively producing propane‐2,2‐diyldicyclohexane (DCHP), a saturated hydrocarbon relevant to jet fuel applications. A multifunctional Ru@P‐CHS(g‐C 3 N 4 ) catalyst integrates light harvesting, electron mediation, acidity, and hydrogen activation, enabling near‐quantitative conversion of bisphenol A with ∼94% molar selectivity toward DCHP. The catalyst also efficiently depolymerizes a range of real‐world PC waste. Mechanistic investigations, including in situ UPS, kinetic isotope effect measurements, H 2 ─D 2 scrambling experiments, and DRIFT‐IR spectroscopy, reveal light‐driven electron accumulation at Ru sites and the formation of Ru─H intermediates, confirming illumination‐induced H 2 activation at Ru that drives C─O bond cleavage. This work establishes a sustainable strategy for converting end‐of‐life plastics into fuel‐range hydrocarbons and introduces reductive photocatalysis as a new paradigm for plastic upcycling.