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Four asymmetric D-π-A-π-A’ visible light initiators (IDs) were synthesized with indole as electron donor (D), carbonyl group and oxime ester as the first and second electron acceptors (A and A’)....

A visible-light-promoted and transition-metal-free photoredox-catalysis strategy is developed for the synthesis of thioxanthone derivatives (TXs). The mechanistic study and density functional theory calculations suggest that visible-light-promoted intramolecular cyclization can be divided into hydrogen atom transfer, C−C formation, and oxidative dehydrogenation with high regioselectivity and reactivity. Significantly, this C−C formation strategy can be used in TXs-based commercial photoinitiators and drugs at the gram level.