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A I2‐DMSO mediated approach to introduce −OCD3 into pyrroles in situ via multicomponent cascade cyclization reaction using methyl ketones, aniline, ethyl benzoylacetate and CD3OD as readily available substrates is reported. This process realizes introduction of −OCD3 into the Hantzsch pyrrole synthesis and synthesis of deuterated alkoxy‐substituted pyrroles with formation of one C−C bond, one C−O...