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In this work, we have developed a simple and very effective experimental strategy for the reaction of Knoevenagel via the condensation of aromatic aldehydes substituted with active methylene compounds in the presence of hybrid nanocomposites xMCl 2 -yNaPO 3 (MCl 2 = 2,2'-dibenzimidazolyl butane dichlorhydrates), under ecological conditions. The Phosphate-Benzimidazole hybrid nanocomposite as heterogeneous catalysts has demonstrated a high catalytic activity for the Knoevenagel condensation in ethanol as an ecological solvent. It has several advantages such as light reaction conditions, a simple and ecological working procedure. Meanwhile, xMCl 2 -yNaPO 3 can be recovered by simple filtration and this catalytic system having an interesting lifetime (five cycles) with no decrease in activity., (© 2020 Published by Elsevier Ltd.)