We determined whether estimation of intake of specific carotenoids with a standard food-frequency questionnaire (FFQ) could be improved by collection of additional data on the intake of carotenoid-rich food items. The foods included on an addendum to the standard FFQ were potentially important dietary contributors of alpha- and beta-carotene, beta-cryptoxanthin, lutein, zeaxanthin, or lycopene. Participants (n = 215), ages 50-74 years, provided fasting blood samples and completed the FFQ and the addendum. The participants were enrolled in a prepaid health plan and had undergone screening sigmoidoscopy for detection of colorectal polyps. Addendum foods were identified that accounted for variation in blood levels of specific carotenoids, conditional on intake of foods on the standard FFQ. Estimated carotenoid intakes from the standard FFQ, and from the modified FFQ with the selected addendum foods, were examined in relation to plasma carotenoid levels. The correlation coefficient between estimated carotenoid intake and plasma levels (adjusted for age, sex, serum cholesterol, alcohol intake, smoking status, and energy intake) were essentially the same for the standard and modified FFQs. The adjusted correlations for the standard FFQ only were 0.26 for alpha-carotene, 0.22 for beta-carotene, 0.36 for beta-cryptoxanthin, 0.32 for lutein+zeaxanthin, and 0.34 for lycopene. Adding carotenoid-rich foods to the FFQ did not improve estimation of intake for the carotenoids examined in this population. We conclude that assessment of intake of specific carotenoids with the FFQs currently in use may not necessarily be improved by a modified list of carotenoid-rich foods.