Measuring dietary intakes in a multi-ethnic and multicultural setting, such as Malaysia, remains a challenge due to its diversity. This study aims to develop and evaluate the relative validity of an interviewer-administered food frequency questionnaire (FFQ) in assessing the habitual dietary exposure of The Malaysian Cohort (TMC) participants. We developed a nutrient database (with 203 items) based on various food consumption tables, and 803 participants were involved in this study. The output of the FFQ was then validated against three-day 24-h dietary recalls (n = 64). We assessed the relative validity and its agreement using various methods, such as Spearman’s correlation, weighed Kappa, intraclass correlation coefficient (ICC), and Bland–Altman analysis. Spearman’s correlation coefficient ranged from 0.24 (vitamin C) to 0.46 (carbohydrate), and almost all nutrients had correlation coefficients above 0.3, except for vitamin C and sodium. Intraclass correlation coefficients ranged from −0.01 (calcium) to 0.59 (carbohydrates), and weighted Kappa exceeded 0.4 for 50% of nutrients. In short, TMC’s FFQ appears to have good relative validity for the assessment of nutrient intake among its participants, as compared to the three-day 24-h dietary recalls. However, estimates for iron, vitamin A, and vitamin C should be interpreted with caution.
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