Meldrum's acid catalyzed the reaction of tetracyanoethylene with aromatic, heteroaromatic, and conjugated aldehydes led to arylidenemalononitrile in water in good yields at 80° C. The work-up of reactions is very simple and the crude products are sufficiently pure to be used without further purification. The procedure provides an alternative method for the synthesis of arylidenemalononitrile.