Background: Alkylresorcinols (ARs), phenolic lipids exclusively present in the outer parts of wheat and rye grains, have been proposed as specific dietary biomarkers of whole-grain wheat and rye intake. Objective: The objective was to validate plasma ARs as a biomarker of whole-grain wheat and rye intakes by studying the correlation between their plasma concentration and intake calculated from food records. Design: In a randomized crossover study, 22 women and 8 men were given a defined amount of either whole-grain or refined-cereal-grain products to be included in their habitual diets for two 6-wk periods. Blood samples were collected and food intakes were recorded before and after each intervention period. Results: Plasma AR concentrations were significantly higher after the whole-grain diet period than after the refined-grain period (P < 0.0001) and were well correlated with average daily AR intake estimated by self-reported weighed food records (Spearman's r = 0.58, P < 0.001). Conclusion: Plasma AR concentrations are correlated with intake assessed by food records, which suggests that ARs are selective nutritional biomarkers for the intake of whole-grain wheat and rye.