Plants existing in nature could be used as source of nutrition and bioactive compounds. Some of the wild and underutilized plants such as African baobab, amaranth, tarragon, Malabar spinach, borage, Ethiopian rape, goosefoot, chicory, spider plant, mallow, sea kale, curcuma, squash, roselle, water spinach, bitter melon, drumstick, tassel hyacinth, prickly pear, parsnip, tomatillo, Indian poke, purslane, yellow cresses, black nightshade, and water leaf are used as vegetables, and some other wild leguminous plants including jack bean, rattlepod, Hausa groundnut, lablab bean, pea vines, subabul, Andean lupin, horse gram, deer-eye bean, stinky bean, winged bean, African yam bean, adzuki bean, bambara groundnut, and rice bean are used for proteins and other nutrients. These plants are sources of nutrients and are also rich in bioactive compounds. Studies carried out during the past several decades have shown that bioactive compounds obtained from the underutilized vegetables and legumes (UVLs) have important role in preventing chronic diseases like cancer, diabetes, and coronary heart diseases. Phytochemicals present in UVLs have demonstrated antioxidant, anticancer, antimicrobial, antihypertensive, anti-inflammatory, and hepatoprotective activities. In the current chapter, we are presenting a review on importance of UVLs, their nutritional value, bioactive compounds, and their biological activities.