Job’s tears (Coix lacryma-jobi) millet is a minor, underexploited, nutrient-rich cereal crop mostly consumed in Asia and other parts of the world. This chapter provides a detailed overview of the chemical composition of Job’s tears, which is widely dependent upon the genotype, environmental conditions, and processing techniques. Key bioactive compounds, proteins, lipids, and minerals that contribute to its nutritional and functional properties are also discussed. Methods of starch isolation from Job’s tears, including both traditional and enzymatic approaches, are examined for their effectiveness and applicability. Additionally, this chapter explores various Job’s tears starch modification techniques aimed at enhancing the physicochemical properties of its starch for diverse applications. Job’s tears is used in traditional medicine to cure various illnesses. Beyond its traditional culinary uses, it finds application in non-food sectors. Modified Job’s tears starch has significant potential in food technology, pharmaceuticals, and biodegradable material production. It is a sustainable crop with broad applicability and emphasizes its role in supporting future advancements and green industry practices.