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A visible‐light‐induced metal‐free catalytic system was developed for the synthesis of arylphosphonates starting from arylhydrazines and trialkylphosphites. By using the inexpensive eosin B as catalyst, sub‐stoichiometric amounts of DABCO, and ambient air as oxidant, diverse arylphosphonates were obtained under visible‐light irradiation. Notably, this catalytic system is suitable for gram‐scale reaction by utilizing sunlight as an illumination source.