A handy new ligand: The CpRu complex (Cp=cyclopentadienyl) of a new type of chiral bisamidine ligand with a naphtho[1,2‐b:7,8‐b′]dipyrroloimidazole (Naph‐diPIM) skeleton with a Brønsted acid efficiently catalyzes dehydrative intermolecular C‐allylation with high enantio‐ and regioselectivity. The catalytic system also gives nearly enantiomerically pure cycloalkanes and N‐ and O‐heterocycles with a substrate/catalyst ratios of up to 10 000.

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N-, and O-Allylation. -The RuCp complex of a new chiral bidentate sp 2 -N ligand is shown to catalyze a variety of intra-and inter-molecular enantioselective dehydrative C-, N-, and O-allylation reactions without the need of extra additives. Water is the only co-product, making the reaction clean and simplifying product isolation. -(MIYATA, K.; KUTSUNA, H.; KAWAKAMI, S.; KITAMURA*, M.; Angew. Chem., Int. Ed. 50 (2011) 20, 4649-4653, http://dx.