A convenient, highly efficient and time economic method has been described for the chemo- and regioselective synthesis of 5-aryloyl-1,3,7,9-tetraalkyl-2,8-dithioxo-2,3,8,9-tetrahydro-1H-pyrano[2,3-d:6,5-dˊ]dipyrimidine-4,6(5H,7H)-diones derivatives by one-pot two-component reaction of 1,3-diethyl-2-thiobarbituric acid or 1,3-dimethyl-2-thiobarbituric acid with substituted arylglyoxalmonohydrates using commercially available zirconium (IV) oxydichloride octahydrate (ZrOCl2.8H2O) as green Lewis acid catalyst. This method is associated with some attractive characteristics such as good selectivity, very short reaction time, high yield of products, cleaner reaction profile, no harmful by-product, cheap and environmental benign catalyst, simple experimental and work-up procedure. This procedure does not require solvent separation and purification steps such as column chromatography.