Iodine is an essential trace element for the synthesis of thyroid hormones, which play an important role in growth and development, metabolism, and body organ function. There is no iodine-specific food frequency questionnaire (I-FFQ) for pregnant women in China. This study aimed to validate and optimize an I-FFQ. A total of 1802 pregnant women were included in this study. The iodine nutrition survey was performed using I-FFQ and 3-day estimated food diary (3DEFD). Seventy-one women of reproductive age repeated the I-FFQ twice to assess for FFQ reproducibility. Further optimization of the I-FFQ was accomplished by integrating iodine contributions to simplified questionnaire items. Correlation and Bland-Altman analyses were used to verify the consistency of I-FFQ with 3DEFD, as well as the stability and feasibility of I-FFQ optimization. The I-FFQ and 3DEFD had a strong correlation (R = 0.76, P < .001) and agreement (Kappa = 0.731, P < .001). A Bland-Altman plot showed that 5.1% of participants exceeded the limit of agreement. Nonpregnant women of reproductive age completed the I-FFQ twice, and the results had a strong correlation (R = 0.72, P < .001). A Bland-Altman analysis showed that 5.6% of individuals were located outside the limit of agreement. The consistency of I-FFQ before and after optimization was good (Kappa = 0.982, P < .001). Therefore, I-FFQ could be used as a valid tool to estimate iodine intake among Chinese pregnant women. The optimized I-FFQ could shorten survey time without affecting its accuracy.