Iodine loss is common in the soil of hilly regions due to higher precipitation rates and steeper slopes. Iodine deficiency in soil reduces iodine’s bioavailability to fruits and vegetables and consequently may contribute to health complications. However, the iodine retention of soils after the addition of selected organic and inorganic amendments has not been studied. Therefore, a study was carried out to investigate iodine loss during surface runoff. For this purpose, a soil amendment (namely, sawdust, charcoal, wood ash, lime or gypsum) was applied separately to pasture and agricultural soils under natural rainfall conditions. The soil was fertigated with iodine in the form of potassium iodide (KI) at the rate of 200 ppm. Surface runoff was related to soil properties. Results showed that iodine content in surface runoff was linearly related with soil pH (R2 = 0.89, p < 0.05) and inversely related with soil organic carbon (R2 = −0.76, p < 0.05). Soils amended with sawdust had significantly reduced iodine content in runoff. A higher amount of iodine was lost via surface runoff from soil after inorganic amendment. Soil amendments were varied for iodine retention in soil in the order of sawdust > charcoal > wood ash > lime > gypsum. The study results indicated that organic amendments, especially sawdust, improved soil properties and increased the iodine retention capacity of soils.