This study assesses the distribution of goiter in the Kalutara District, Sri Lanka in order to find causative factors for the occurrence of goiter even after the salt iodization. A questionnaire survey was conducted at the household level and at the same time iodine and selenium levels of the water sources were analyzed. Questionnaire survey results indicated the highest numbers of goiter patients in the northern part where the lowest were found in the southern sector which may be due to the presence of acid sulfate soils. Females were more susceptible and it even showed a transmittance between generations. Average iodine concentrations in subsurface water of goiter endemic regions are 28.25 ± 15.47 μg/L whereas non-goiter regions show identical values at 24.74 ± 18.29 μg/L. Surface water exhibited relatively high values at 30.87 ± 16.13 μg/L. Endemic goiter was reported in some isolated patches where iodine and selenium concentrations low, latter was <10 μg/L. The formation of acid sulfate soils in the marshy lands in Kalutara district may lead to transformation of biological available iodine oxidation into volatile iodine by humic substances, at the same time organic matter rich peaty soil may have strong held of iodine and selenium which again induced by low pH and high temperature were suggested as the instrumental factors in the endemic goiter in Kalutara district. Hence, geochemical features such as soil pH, organic matter and thick lateritic cap in the Kalutara goiter endemic area play a role in controlling the available selenium and iodine for food chain through plant uptake and in water.