3,4-Dihydropyrimidin-2(1H)-one derivatives were synthesized using layered alpha-zirconium sulfophenylphosphonate as a recyclable heterogeneous catalyst. Several classes of reagents, such as functionalized aromatic and aliphatic aldehydes, beta-dicarbonyl derivatives and 2-aminobenzimidazole, were used to synthesize different 3,4-dihydropyrimidin-2(1H)-one derivatives under solvent free conditions.