Catalytic Photoactive Ternary Electron Donor–Acceptor Complex Enabled Synthesis of Isoquinoline‐1,3(2H,4H)‐Diones

Tuning multiple noncovalent interactions to form multicomponent photoactive electron donor−acceptor (EDA) complexes for driving chemical reactions presents significant challenges yet holds profound implications. Hantzsch ester (HE) is recognized as an exceptional EDA donor, while it typically forms binary EDA complexes requiring stoichiometric amounts. Ternary EDA complexes involving HE in catalytic EDA systems remain scarce. Herein, we developed a H‐bonding‐assisted catalytic ternary EDA complex strategy employing HE for the synthesis of diverse isoquinoline‐1,3(2H,4H)‐diones. This operationally simple, visible‐light‐mediated platform efficiently converted primary, secondary, and tertiary carboxylic acids‐derived NHP esters into structurally diverse alkylated isoquinoline‐1,3(2H,4H)‐diones.