Taro (Colocasia esculenta L.) is one of the underutilized roots and tuber crops that have the potential to be used as a future smart food to combat malnutrition and hunger in several parts of the world. Taro is one of the world’s oldest domesticated crops and belongs to the Araceae family, which contains 106 and 2500 genera and species, respectively. Nigeria, China, Cameroon, Ghana, and Papua New Guinea are the World’s top taro-producing countries. Taro leaves and stems are the main by-products with promising potential applications. The leaves are rich in proteins, dietary fiber, and micronutrients and low in calories. Several antinutrients (tannins, phytates, and oxalates) are present in these by-products, limiting their wide use in the same way for the taro corms. Alkaloids, flavonoids (catechin, kaempferol, orientin, rutin, quercetin, and vicenin), saponins, sterols, phenolic acids (caffeic, gallic, benzoic, chlorogenic, and ellagic acids), and lectins (tarin) are the main bioactive phytochemicals from taro’s by-products with antiatherogenic, antimicrobial, antioxidant, antidiabetic, anticarcinogenic, antihypertensive, and insecticidal, hepatoprotective, immunoprotective, and neuroprotective properties. Taro by-products have several food applications in the production of gluten-free noodles, bread, and extruded snacks, as well as non-food applications in bioethanol and pharmaceuticals. Gastronomic applications for taro leaves include making traditional dishes and various value-added food products such as purees, sauces, stews, and soups with enhanced nutritional and sensory characteristics. This chapter presents the latest highlights on Taro’s by-products, bioactives, potential applications, health benefits, and biological activities.