Here an unprecedented formal deformylative phosphonylation is disclosed. Under the catalysis of 1 mol % 1,2,3,5-tetrakis(diphenylamino)-4,6-dicyanobenzene (4DPAIPN) and the presence of 200 mol % triethylamine as additive, 4-alkyl-1,4-dihydropyridines (DHPs), derived from aldehydes, underwent phosphonylation smoothly with 9-fluorenyl o-phenylene phosphite, allowing facile synthesis of alkylphosphonates. This strategy is applicable to primary, secondary, and even tertiary DHPs, and exhibits a broad substrate scope and excellent functional group tolerance, thereby enabling the late-stage phosphonylation of a series of naturally-ocurring bioactive and biorelevant molecules.

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