In this study, a flexible multifunctional fibrous membrane for heterogeneous Fenton-like removal of organicand pathogenic contaminants from wastewater was developed by immobilizing zerovalent ironnanoparticles (Fe-NPs) on an amine/thiol grafted polyester membrane. Full characterization of theresulting polyester membranes allowed validation of successful grafting of amine/thiol (NH2 or SH)functional groups and immobilization of Fe-NPs (50–150 nm). The Fenton-like functionality of ironimmobilized fibrous membranes (PET–Fe, PET–Si–NH2–Fe, PET–NH2–Fe, and PET–SH–Fe) in thepresence of hydrogen peroxide (H2O2) was comparatively studied in the removal of crystal violet dye(50 mg L1). The effect of pH, amount of iron and H2O2 concentration on dye removal wassystematically investigated. The highest dye removal yield reached 98.87% in 22 min at a rate constant0.1919 min1 (R2 ¼ 95.36) for PET–SH–Fe providing 78% toxicity reduction assessed by COD analysis.These membranes could be reused for up to seven repeated cycles. Kinetics and postulated mechanismof colour removal were proposed by examining the above results. In addition, the resultant membranesshowed substantial antibacterial activity against pathogenic bacteria (Staphylococcus epidermidis,Escherichia coli) strains studied through disc diffusion-zone inhibitory and optical density analysis. Thesefindings are of great importance because they provide a prospect of textile-based flexible catalysts inheterogeneous Fenton-like systems for environmental and green chemistry applications.