Iodine excess typically affects thyroid function in the human body and may damage carotid artery. Four investigation plots with different water iodine levels were selected in Shandong Province, China. These included a low, medium, and high iodine group and an iodine excess group whose water iodine content was < 10, 50–150, 150–300, and > 300 μg/L, respectively. Residents aged 20–65 years answered a questionnaire and underwent carotid artery ultrasonography, and their height, weight, and urinary iodine concentrations were measured. A total of 2026 individuals participated in the study. Urinary iodine concentration increased with increased water iodine levels. The medial thickening rate and intimal roughness rate in the iodine excess group were significantly higher than in the other three groups. After controlling for factors such as gender, age, and BMI, iodine excess remained as a risk factor for carotid intima-media thickening. Excess water iodine in the external environment is a risk factor for intima-media thickening of the carotid artery, suggesting that iodine excess may cause vascular injury and promote atherosclerosis.