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Copper(I) complexes containing acylthio‐ and selenoureato ligands can be accessed either by transmetallation from the corresponding silver compounds or by direct reaction of the acylthio/selenourea with a copper(I) precursor in the presence of base. Several examples of tricoordinate organocopper(I) complexes containing N‐heterocyclic carbenes as well as tetrahedral bis(phosphane) copper(I) compounds...