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Abstract Photoinduced initiators for continuous activator regeneration atom transfer radical polymerization (PICAR ATRP) using sodium pyruvate and blue light (λ_max = 456 nm) is reported. Water‐soluble oligo(ethylene oxide) methyl ether methacrylate (OEOMA₅₀₀) was polymerized under biologically relevant conditions. Polymerizations were conducted with 1000 ppm (with respect to the monomer) concentrations of CuBr₂, tris(2‐pyridylmethyl)amine, and 1000 ppm or less FeCl₃as a cocatalyst in water. Well‐defined polymers with up to 90% monomer conversion, high molecular weights (M_n > 190,000), and low dispersity (1.14 < Ð < 1.19) were synthesized in less than 60 min. The polymerization rate and dispersity were tuned by varying the concentration of sodium pyruvate (SP), iron, and supporting halide, as well as light intensity. The Cu/Fe dual catalysis provided oxygen tolerance enabling rapid, well‐controlled, aqueous PICAR ATRP of OEOMA₅₀₀without deoxygenation.