Iodine is the main constituent of thyroid hormones, which in turn are required for fetal brain development. However, the relation between iodine intake during pregnancy, thyroid function, and child neurodevelopment needs further evaluation. The authors assessed the association of maternal iodine intake from diet and supplements during pregnancy and of maternal and neonatal thyroid function with infant neurodevelopment. The Mental Development Index and Psychomotor Development Index (PDI) for 691 children were obtained between 2005 and 2007 using the Bayley Scales of Infant Development at age 1 year in a prebirth cohort in Valencia, Spain. In multivariate analyses, a maternal thyrotropin level >4 μU/mL was associated with an increased risk of a PDI <85 (odds ratio = 3.5, P = 0.02). Maternal intake of ≥150 μg/day, compared with <100 μg/day, of iodine from supplements was associated with a 5.2-point decrease in PDI (95% confidence interval: -8.1, -2.2) and a 1.8-fold increase in the odds of a PDI <85 (95% confidence interval: 1.0, 3.3). When analyses were stratified by sex, this association was intensified for girls but was not observed for boys. Further evidence on the safety and effectiveness of iodine supplementation during pregnancy is needed before it is systematically recommended in iodine-sufficient or mildly deficient areas.