For over 40 years, food-matrix certified reference materials (CRMs) have been available for determination of trace element content, and a wide variety of materials are available from most producers of CRMs. However, the availability of food-matrix CRMs for organic nutrients has been more limited. The European Commission (EC) Bureau Communautaire de Référence (BCR) and the National Institute of Standards and Technology (NIST) introduced food-matrix CRMs with values assigned for vitamins and other organic nutrients such as fatty acids and carotenoids in the 1990s. The number of organic nutrients for which values were assigned has increased significantly in the past decade, and the approach and analytical methods used for assignment of the certified values have also evolved. Recently, dietary supplement-matrix CRMs such as multivitamin tablets with values assigned for vitamins and carotenoids, and fish and plant oils with values assigned for fatty acids have appeared. The development, evolution, and improvement of food- and dietary supplement-matrix CRMs for determination of vitamins, carotenoids, and fatty acids are described, with emphasis on CRMs made available in the past 10 years. Recent food and dietary supplement CRMs for the determination of organic nutrients include infant formula, multivitamin tablets, milk and egg powders, breakfast cereal, meat homogenate, blueberries, soy flour, fish and plant oils, dry cat food, and protein drink powder. Many of these food- and supplement-matrix CRMs have values assigned for over 80 organic and inorganic nutrients, toxic elements, proximates, and contaminants. The review provides a critical assessment of the challenges and evolving improvements in the production and the analytical methods used for value assignment of these CRMs. The current status and future needs for additional food- and dietary supplement-matrix CRMs for organic nutrients are also discussed.