Following a nuclear accident, radioactive iodine causes great concern to public health and safety. Organic iodide, because of its ability to escape reactor containment building and high environmental mobility, constitutes a predominant fraction of airborne radioiodine at places far away from the accident site. As the iodine released from a reactor core is inorganic iodine, it is vital to understand the mechanism of organic iodide formation inside reactor containment. In this context, we investigated the surface prevalence and adsorption of various inorganic iodines, I-, I-3(-), and IO3-, at a nuclear paint (used in nuclear installations) monolayer-water interface, mimicking the painted inner walls of an accident-affected containment building that are exposed to the iodine-containing condensed water layer. Vibrational sum frequency generation (VSFG) measurements in the OH and CH stretch regions reveal that the paint-water interface changes its charge characteristics with the pH of the water that affects the degree of interaction with the iodine species. At the acidic condition (bulk pH < 7), the paint becomes positively charged and strongly adsorbs the negatively charged iodine species dissolved in the aqueous phase, whereas at the alkaline condition (bulk pH > 9.5), the paint becomes net neutral and weakly interacts with the iodine species. These interactions change the conformation of the paint such that its hydrophobic alkyl groups orient increasingly away from the aqueous phase. The order of adsorption increases as IO3- < I- < I-3(-) for the different iodine species studied.