The objective of this study is to demonstrate the efficiency of the containment spray system on the removal of iodine from atmosphere under environmental conditions expected in a reactor accident. As a small-scale vessel simulating a reactor containment, we used two types of steel vessels: one is made of mild steel with the interior surface painted; the other is made of stainless steel. Both tanks are 1.5 m diam × 3 m high. The removal rates of iodine with and without sprays were measured as functions of spray system conditions such as temperature, pressure, spray flow rate, and spray solution. The removal rates were evaluated from the variation for iodine concentration in the gas phase, which was determined by means of the thiosulfate titration method for elemental iodine and gas-liquid chromatographic techniques for organic iodides.