Abstract: The efficient construction of C= N double bonds has been achieved by the Ir- catalyzed intramolecular acceptorless dehydrogenative cross-coupling of tertiary amines and amides. An iridium/2-hydroxypyridine complex was identified as the highly efficient catalyst. A number of quinazolinone derivatives was prepared in excellent yields. An iridium- mediated CÀH activation mechanism is proposed. This finding provides an ...