A one-pot method for the synthesis of six novel 5-aryl-1,3-dimethyl-7-selenoxopyrimidino[4,5- d]pyrimidine-2,4(1 H,3 H)-diones in excellent yields at room temperature has been achieved via reaction between potassium selenocyanate and an aroyl chloride followed by the addition of 6-amino- N,N′-dimethyluracil.