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An efficient four-component reaction to synthesize pyrrolo[2,1-a]isoquinolines from malononitrile, aromatic aldehydes, isoquinoline, and cyclohexyl isocyanide under solvent-free conditions is described. In a convenient, simple, and efficient one-pot procedure, the domino Knoevenagel-nucleophilic cycloaddition reaction affords excellent yields of products in less than 1 h.