Nowadays, consumers are more conscious of the environmental and nutritional benefits of foods. Pseudocereals grains, edible seeds belonging to dicotyledonous plant species, are becoming a current trend in human diets as gluten-free (GF) grains with excellent nutritional and nutraceutical value. Pseudocereals are a good source of starch, fiber, proteins, minerals, vitamins, and phytochemicals such as saponins, polyphenols, phytosterols, phytosteroids, and betalains with potential health benefits. The present review aims to summarize the nutritional quality and phytochemical profile of the three main pseudocereal grains: quinoa, amaranth and buckwheat. In addition, current evidence about their health benefits in animal models and human studies is also provided in detail. Based on the accumulating research supporting the inclusion of pseudocereals grains in the diet of celiac persons, this review discusses the recent advances in their application for the development of new GF products. Future directions for a wider cultivation and commercial exploitation of these crops are also highlighted.