The growing global emphasis on health has boosted interest in leaf-derived bioactive compounds rich in dietary fiber, phenolics, vitamins, and antioxidants associated with protective effects against cancer, inflammation, and cardiovascular diseases. Soluble (such as pectin, inulin) and insoluble (such as cellulose, lignin) dietary fibers are responsible for the enhancement of gut microbiota, regulation of body weight, and reduction in mortality risk, and their leaf extraction is a prerequisite for food and pharmaceutical industries. This chapter presents an enzymatic-gravimetric method for isolating total dietary fiber from leaf material, addressing the need for green and efficient extraction techniques. It involves enzymatic hydrolysis in a sequential fashion by heat-stable α-amylase, protease, and amyloglucosidase on dried leaves, followed by precipitation and filtration processes to determine the fractions of insoluble, soluble, and total dietary fiber content. The method ensures maximum yield with integrity of compounds ensured and involves green chemistry principles of reducing the use of chemicals. The major steps include preparation of the sample at 60–70 °C, incubation at pH-controlled conditions, and analysis of protein and ash residue content, thus making the quantitation of the fiber more accurate. Overall, this process encourages sustainable harvesting, offering an avenue for the development of health-enhancing leaf-based nutraceuticals and augmenting nutrition security worldwide.