The one-pot synthesis of noble series of 1,2,4-triazines was investigated from the reactions of semicarbazide or thiosemicarbazide with various α,β-dicarbonyl compounds under reflux conditions in EtOH-H2O (9:1) mixture as a solvent by the nano-sized silica-supported FeCl3 (FeCl3@SiO2). To find out the adsorption capacity, the FeCl3 content of the catalyst was measured via the atomic adsorption technique. The reactions were completed with high yields of the products and the catalyst easily separated and re-used for successive reaction runs without the significant loss of activity.