In the present study, Ni/Fe nanoparticles were synthesized using bound micelles as a template and 3, 3 0 , 4, 4 0 -tetrachlorobiphenyl (PCB77) as the target contaminant. The dual bound micelles, which are composed of polyvinylpyrrolidone (PVP) and sodium dodecyl sulfate (SDS), were found to be superior to single-component templates for the dispersion of metallic ions and thus directed the synthesis of Ni/Fe nanoparticles with improved properties. After characterization of the di®erent nanoparticles, it was found that the sustained e®ectiveness of PVP-SDS bound micelles a®orded specialized structures with two gradations of Ni/Fe nanoparticles, correlating to more active sites and higher activity. The improved activity of the Ni/Fe nanoparticles was nally exhibited by the higher ratio (99.3% in 72 h) and e±ciency (k obs of 0.0674 h À1 ) of PCB77 removal. Herein, the utilization of PVP-SDS bound micelles is proposed as a template for the improvement of iron-based nanoparticles and correlated research.