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Objective: To design and validate a literature-derived, population-based Children’s Dietary Inflammatory Index (C-DII)TM. Design: The C-DII was developed based on a review of literature through 2010. Dietary data obtained from children in 16 different countries were used to create a reference database for computing C-DII scores based on consumption of macronutrients, vitamins, minerals, and whole foods. Construct validation was performed using quantile regression to assess the association between C-reactive protein (CRP) concentrations and C-DII scores. Data Sources: All data used for construct validation were obtained from children between six and 14 years of age (n = 3300) who participated in the U.S. National Health and Nutrition Examination Survey (NHANES) (2005–2010). Results: The C-DII was successfully validated with blood CRP concentrations in this heterogeneous sample of 3300 children from NHANES (52% male; 29% African American, 25% Mexican American; mean age 11 years). The final model was adjusted for sex, age, race, asthma, body mass index (BMI), and infections. Children in level 3 (i.e., quartiles 3 and 4 combined) of the C-DII (i.e., children with the most pro-inflammatory diets) had a CRP value 0.097 mg/dL higher than that in level 1 (i.e., quartile 1) for CRP values at the 75th percentile of CRP using quantile regression (p < 0.05). Conclusion: The C-DII predicted blood CRP concentrations among children 6–14 years in the NHANES. Further construct validation with CRP and other inflammatory markers is required to deepen understanding of the relationship between the C-DII and markers of inflammation in children.