As a new attempt to control iodine deficiency disorder (IDD), we explored a method of iodine supplementation by raising the iodine content in vegetables. When grown in the soil supplemented with iodized fertilizer, the three experimental plant species (cucumber, aubergine, and radish) show increasing iodine levels in both leaf and fruit/rhizome tissues as the iodine content added in soil increases. Excessive iodine added to soil can be toxic to plants, whereas the tolerance limit to excessive iodine varies in the three plant species tested. The migration and volatilization of iodine in soil is correlated with the properties of the soil used. The residual iodine in soil increases as the iodine added to soil increases. The diatomite in the iodized fertilizer helps to increase the durability of the iodized fertilizer. This study potentially provides a safe and organic iodine supplementation method to control IDD.