As the scope of radiation use in medical and industrial fields has expanded, interest in radiation shielding is increasing. Most existing radiation shields use Pb-based products, primarily in the form of a laminated sheet, which requires attention as fine cracks may occur depending on the usage and storage conditions. The weight of the sheets limits users’ activities, and they pose a risk of heavy metal contamination. To address these problems, this study proposed a shielding fiber with improved flexibility and workability, and thus, produce a shielding garment. Masterbatches of polyethylene terephthalate (PET) fiber were manufactured using the eco-friendly materials, BaSO4 and Bi2O3. Yarns were fabricated by the melt spinning process, and fabrics were woven. With 5 wt% of shielding material, the yarns’ shield against radiation and was sufficiently strong for fabric weaving. The fibers’ radiation shielding averaged 9–13%, with the Bi2O3 fiber displaying better shielding performance than the BaSO4. It is believed that the findings of this study on improving the yarn manufacturing process could be applied for protection against low-dose and scattered rays in medical applications and for aerospace radiation protection. In addition, the proposed shielding fibers’ flexibility makes them suitable for future use in the production of various radiation shields.