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We have described the catalytic activities of dicalcium phosphate dihydrate (DCPD) in the condensation reaction of various substituted benzaldehydes with active methylene compound malononitrile. The influences of reaction conditions on the corresponding catalytic behavior have been investigated. The results showed that the DCPD exhibited high catalytic activity and versatility and that it can be recycled without significant loss of its activity for the condensation reactions, which shows the material is a promising new type of heterogeneous catalyst for the condensation reactions. Meanwhile, the catalytic results of DCPD compared favorably with those of other materials for Knoevenagel reactions reported previously.