A 2014 national assessment of salt iodization coverage in Cambodia found that 62% of samples were non-iodized, suggesting a significant decline in daily iodine intakes. The Cambodian Micronutrient Survey conducted in 2014 (CMNS-2014) permitted obtaining national data on urinary iodine concentrations (UIC) to assess iodine status and whether iodized salt use had an impact. Urine samples were collected from mothers (n = 736) and children (n = 950). The median UIC was 63 µg/L and 72 µg/L in mothers and children respectively. More than 60% of mothers and their children had a UIC < 100 µg/L, thereby indicating a serious public health problem. Iodine status was significantly lower among mothers and children living in rural areas, belonging to the poorest socioeconomic category, or living in a household not using iodized salt. The limited enforcement of the legislation for iodized salt has resulted in a major decrease in the prevalence of iodized salt, which in turn has compromised iodine status in Cambodia. It is essential for the government to enhance enforcement of the iodized salt legislation, and implement short term strategies, such as iodine supplementation, to prevent an increase of severe complications due to iodine deficiency in the Cambodian population.