Over the past decades, an enormous body of literature dealing with the natural deposition of carotenoids in plant- and animal-based foods has accumulated. Prominent examples are the large solid-crystalline aggregates in carrots and tomatoes or the lipid-dissolved forms in dairy products and egg yolk. Latest research has identified lipid-dissolved forms in a rare number of plant foods, such as tangerine tomatoes and peach palm fruit (Bactris gasipaes Kunth). In addition, liquid-crystalline forms were assumed in so-called tubular chromoplasts of numerous fruits, e.g., in papaya, mango, and bell pepper. The bioavailability of carotenoids from fresh and processed foods strongly depends on their genuine deposition form, since their effective absorption to the human organism requires their liberation from the food matrix and subsequent solubilization into mixed micelles in the small intestine. Consequently, a broad overview about the natural array of carotenoid deposition forms should be helpful to better understand and modulate their bioavailability from foods. Furthermore, naturally highly bioavailable forms may provide biomimetic models for the improved formulation of carotenoids in food supplements. Therefore, this review paper presents scientific evidence from human intervention studies associating carotenoid deposition forms with their bioavailability, thus suggesting novel technological and dietary strategies for their enhanced absorption.