The validity coefficient of dietary questionnaire measurements can be estimated from a triangular comparison between questionnaire, reference, and biochemical marker measurements with the method of triads. The method assumes that the measurements are linearly related to true intake and have independent random errors. We applied the method of triads to examples from the European Prospective Investigation into Cancer and Nutrition. In some examples, Heywood cases occurred, ie, the estimated validity coefficients were > 1 or the validity coefficients were not estimable. Such results are caused by random sampling fluctuations or violation of the model assumptions. One possible violation is a positive correlation between the random errors of questionnaire and reference measurements. We used a bootstrap method to estimate CIs for the validity coefficients. Validity studies with several hundred subjects, more accurate biochemical indicators of dietary intake, or both, are needed to estimate validity coefficients precisely and avoid complications with the bootstrap method.