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Concise and efficient six-component and four-component domino approaches to anti-1,2-diarylethylbenzamides and highly substituted 2-(2′-azaaryl)imidazoles have been developed under solvent-free and microwave-irradiation conditions. The reactions showed a broad scope of substrates in which a wide range of common commercial aromatic aldehydes and heteroaryl nitriles can be used. The syntheses were finished within short periods (15−34 min) with good to excellent chemical yields and stereoselectivity that avoided tedious workup isolations. New mechanisms involving an umpolung have been proposed for these two reaction processes.