Triphenylammonium tricyanomethanide (Ph3NH)[C(CN)3] was synthesized and used as an efficient and recyclable nanostructured molten-salt (NMS) catalyst for the synthesis of N-benzylidene-2-arylimidazo[1,2-a]pyridin-3-amines by the reaction of various (het)aryl aldehydes with trimethylsilyl cyanide and pyridin-2-amine under solvent-free conditions at 50 °C. The NMS catalyst could be simply recycled and reused several times without significant loss of its catalytic activity.