A synthesis of novel bis(pyrido[2,1‐a]isoquinoline‐1,3‐dicarbonitriles) by the multicomponent reaction of 2‐(6,7‐dimethoxy‐3,4‐dihydroisoquinolin‐1‐yl)acetonitrile with the corresponding bis(aldehydes) and malononitrile in the presence of basic catalysts was reported.