4-Dihydropyrimidin-2(1H)-one derivatives were synthesized using layered α-zirconium sulfophenylphosphonate as a recyclableheterogeneouscatalyst. Several classes of reagents, such as functionalized aromatic and aliphatic aldehydes, β-dicarbonyl derivatives and 2-aminobenzimidazole, were used to synthesize different 3,4-dihydropyrimidin-2(1H)-one derivativesundersolventfree conditions.Graphical Abstract