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Atom Economy: A palladium-catalyzed atom-transfer reaction of secondary alkyl iodides is described. An intramolecular double insertion of an alkyne and olefin provides access to primary iodides possessing β-hydrogen atoms. The process delivers these complex bicyclic homoallylic iodides with tetrasubstituted olefins from easily accessible aliphatic iodides. Different functional groups, including common heterocycles, are tolerated. DOI: 10.1002/anie.201308534