Abstract: | A unified strategy for nickel(0)‐catalyzed C−H allylations, alkenylations, and dienylations has been realized through versatile hydroarylations of allenes with ample scope. Thus, an inexpensive nickel catalyst modified with a N ‐heterocyclic carbene ligand enabled the direct transformation of C−H bonds of biologically relevant imidazole and purine derivatives with full control of regio‐ and chemoselectivity. |