Abstract A series of nineteen benzimidazoles were prepared from ortho-nitroanilines by one- pot transfer hydrogenation, condensation, and dehydrogenation enabled by the concurrent use of two heterogeneous catalysts: montmorillonite-K10 and Pd/C. This strategy was further employed to accomplish a five-step, three-component synthesis of an antifungal benzimidazoquinazoline by using a simple one-pot procedure.