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An eco-friendly and economical approach was proposed to enhance the dyeability of synthetic fabrics with natural dyes, namely curcumin and saffron dyes, by pretreatment using EB irradiation. The approach facilitated the successful dyeing of synthetic fabrics with natural dyes. (EB) irradiation technology is an advanced approach to efficiently modify the physical and chemical properties of polymer materials. This study was based on the pretreatments of PP, nylon 6, and PET by EB irradiation at different doses and oxidation times in the air. The dyeing procedure exhibited excellent coloration behavior and features, commercially acceptable leveling properties. The color fastness and durability tests of the dyed samples achieved excellent ratings. The action of electron beams on the synthetic fabrics afforded new active functional groups, such as the carboxylate groups, which improved the physical and chemical properties of the fibers. These findings could contribute to the development of chemical reactions between fibers and natural dyes to achieve outstanding fastness while maintaining their mechanical properties.