A copper(I)-catalyzed domino reaction of N-(2-benzimidazolyl)-2-aminobenzamide and 2-halogenated benzaldehyde has been studied. The procedure is based on a sequential CuI-catalyzed Ullmann reaction (C鈥揘 bond formation) and two bond cleavage reactions and provides an efficient strategy for the synthesis of benzimidazo[1,2-a]quinazolines catalyzed by CuI/l-proline.