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Abstract Intramolecular methyl–methyl coupling on Au (111) is explored as a new on-surface protocol for edge extension in graphene nanoribbons (GNRs). Characterized by high-resolution scanning tunneling microscopy, noncontact atomic force microscopy, and Raman spectroscopy, the methyl–methyl coupling is proven to indeed proceed at the armchair edges of the GNRs, forming six-membered rings with sp3- or sp2-hybridized carbons.