The danger from the content of dyes produced by textile-industry waste can cause environmental degradation when not appropriately treated. However, existing waste-treatment methods have not been effective in degrading dyes in textile waste. Zero-valent iron (ZVI), which has been widely used for wastewater treatment, needs to be developed to acquire effective green production. Tea (Camellia sinensis) leaves contain many polyphenolic compounds used as natural reducing agents. Therefore, this study aims to synthesize ZVI using biological reducing agents from tea-leaf extract and apply the Fenton method to degrade the color mixture of rhodamine B and methyl orange. The results show that the highest polyphenols were obtained from tea extract by heating to 90 °C for 80 min. Furthermore, PSA results show that ZVI had a homogeneous size of iron and tea extract at a volume ratio of 1:3. The SEM-EDS results show that all samples had agglomerated particles. The ZVI 1:1 showed the best results, with a 100% decrease in the color intensity of the dye mixture for 60 min of reaction and a degradation percentage of 100% and 66.47% for rhodamine B and methyl orange from LC-MS analysis, respectively. Finally, the decrease in COD value by ZVI was 92.11%, higher than the 47.36% decrease obtained using Fe(II).