An organic-zeolite hybrid catalyst was synthesised via solid-state impregnation of the zeolite with an amount of melamine corresponding to 20 mol% of the aluminium content. A high density of basic sites is formed in the zeolite. From infrared spectroscopy and TGA measurements we infer that melaminium cations are formed in the zeolite which are highly thermally stable. IR spectroscopic and TGA measurements showed the presence of melaminium after pre-treatment in vacuum at 450 degrees C. The catalyst exhibited activity in the Knoevenagel condensation reaction between benzaldehyde and ethyl cyanoacetate which is suggested to be promoted by the presence of acid and base sites. The catalyst activity was compared with other known base catalysts including hydrotalcites and magnesium oxide on alumina support. Crown Copyright (C) 2011 Published by Elsevier Inc. All rights reserved.