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Synthesis of 3,4‐pyrroline derivatives via visible‐light‐induced hydro/oxyimination of unactivated olefins is reported. In the presence of the photoredox catalyst fac‐Ir(ppy)3, the key iminyl radical intermediate can be readily generated from O‐acyl oximes, and undergoes intramolecular cyclization and H‐ion from solvent or is trapped by TEMPO to give the corresponding hydro/oxyimination product, respectively. Mechanistic investigations indicate that N,N′‐dimethylpropylene urea (DMPU) works as both reducing agent for catalyst regeneration and H‐donor for product formation in this process.