Direct Dehydrogenative Access to Unsymmetrical Phenones

The first non‐directed dehydrogenative phenone coupling method of methylarenes with aromatic C−H bonds, displaying a large substrate scope, is herein reported. This reaction represents a far more direct atom‐ and step‐efficient alternative to the classical Friedel–Crafts or Suzuki–Miyaura derived acylation reactions. The method can be carried out on a gram scale and was successfully applied to the synthesis of several Ketoprofen drug analogues.