This study reports the synthesis, immobilization and stabilization of multiscale zero valent iron (Fe-0 = ZVI) particles on fibrous polyester (PET) nonwoven membrane for heterogeneous Fenton-like removal of hazardous pollutants in water. Activation of PET fiber surface by air atmospheric plasma with or without a consecutive grafting of hyperbranched poly-(ethyleneglycol)-pseudo generation 5 dendrimer having hydroxyl (-OH) end group functionality created polar reactive functional groups allowing immobilization and stabilization of ZVI particles. Synthesis of ZVI was carried out through chemical reduction of ferric ions, either through a single step in-situ, or a two-step ex-situ reduction-immobilization method. The nonwovens were characterized using wettability, Fourier transform infrared spectroscopy (FTIR), optical microscopy, scanning electron microscopy (SEM), X-ray energy-dispersive spectroscopy (EDS), X-ray diffraction (XRD) and thermo-gravimetric analysis (TGA). Results confirmed the formation and immobilization of nano to sub-micronic multi-scale ZVI particles. The particle size, distribution and stability of ZVI were found to be influenced by the methods of ZVI synthesis and PET surface activation used. The ZVI particles initially formed, quasi-instantaneously turned to yellowish brown indicating the formation of oxide layer, except in the case of dendrimer grafted PET, where higher content (22.30%) and stability of ZVI was detected. All ZVI immobilized nonwovens exhibited high effectiveness towards Fenton-like degradation of malachite green dye (20 ppm), with fastest color removal (98% in 20 min) achieved by dendrimer/ex-situ nonwoven. This nonwoven could be used up to eight repeated cycles providing low TDS (52 ppm) and high COD reduction (66.23%). Combined use of eco-friendly plasma and dendrimer grafting, provides efficient fibrous textile base heterogeneous catalysis.