Acrylamide is present in mainstream cigarette smoke and in some foods prepared at high temperatures. Animal studies have shown that acrylamide exposure alters thyroid function; however, it is not known if this also occurs in humans. The study examined the association between the urinary levels of the acrylamide metabolite and serum thyroid measures in adolescents and young adults. We recruited 793 subjects (mean age, 21.3 years; range, 12–30 years) from a population-based sample of Taiwanese adolescents and young adults to determine if the urinary levels of the acrylamide metabolite N-acetyl-S-(propionamide)-cysteine (AAMA) and the 6 serum thyroid measures are associated. The mean (SD) AAMA were 76.54 (76.42) μg/L. Linear regression analyzes showed a 1-unit increase in natural log AAMA was significantly associated with a decrease in serum free thyroxine (T4) (ng/dL) (β=−0.041, SE=0.013, p=0.001) after controlling for covariates. Subpopulation analyzes showed AAMA and free T4 were significantly associated with females, age 20–30 years, non-current smokers, and non-alcohol consumers. In conclusion, higher urinary AAMA concentrations were associated with decreased levels of free T4 in this cohort. Further studies are warranted to determine if there is a causal relationship between acrylamide exposure and thyroid function.