Using Food Frequency Questionnaires (FFQs) to compare dietary references for screening has been in high demand. However, FFQs have been widely used for ranking individuals in a population based on their dietary intake. We determined the validity of sodium (salt equivalent) intake, potassium intake, and sodium-to-potassium (Na/K) ratio obtained using the FFQ for identifying individuals who deviated from the dietary reference intakes (DRIs) measured using multiple 24-h urinary excretion measurements or 12-day weighed food records (WFR). This study included 235 middle-aged subjects. The correlation coefficients (CCs) between the FFQ and WFR estimates were mostly moderate (0.24−0.54); the CCs between the FFQ and 24-h urinary excretion measurements were low or moderate (0.26−0.38). Values of area under the receiver-operating curve (AUC) at the point of DRIs for salt equivalent or potassium were >0.7 with the WFR as the reference standard and 0.60−0.76 with the 24-h urinary excretion as the reference standard. Using both standard measures, the AUC for the Na/K ratio was <0.7. The accuracy of salt equivalent and potassium intake estimation using the FFQ to determine absolute intake point was comparable to that using WFR, allowing for quantified error, but not as good as that of 24-h urinary excretion.