The potential of Fe(II)-orthophenatrolin, as doped with synthetic zeolite Y nanocluster (Na-Y) via complexation process, after wet impregnation of parent zeolite with FeSO 4 aqueous solution, was studied as a photocatalyst in decolorization of Methyl Green (MG) under UV irradiation. The characterization of the synthesized zeolite nanocluster and the prepared catalyst was studied using X-ray powder diffraction (XRD), infrared spectroscopy (FT-IR), thermal analysis, and SEM methods. The dye photodecolorization process was studied considering the influence of experimental parameters and it was observed that photoreactivity of the photocatalyst was varied with catalyst amount, initial dye concentration, pH of dye solution, temperature, and the presence of KBrO 3 . The optimal experimental parameters were obtained as follows: catalyst amount: 1 gL −1 , dye concentration: 40 ppm, pH: 9, and active component value: 100 mg Fe(II)-orthophenatrolin per g catalyst. The reusability of the intended catalyst was also investigated. The degradation process obeyed first-order kinetics.2 International Journal of Photoenergy metal ions in their higher oxidation state, as Fe(III) and Cu(II), undergo readily photoreduction to Fe(II) and Cu(I), respectively, which is accompanied by oxidation of the organic ligand, or other sacrificial donors. Thus, the environmental photochemistry of the transition metal complexes with organic ligands has a crucial importance for the pollution abatement because it may cause the photodegradation of persistent pollutants, such as phenol and its derivatives or EDTA and related aminopolycarboxylic acids [11,12]. The mechanism of the photocatalysis by the transition metal complexes in a homogeneous phase has been described in [13].Generally, the environmental Fe compounds are classified into two groups, the hydroxo species and chelate complexes, depending on the nature of their ligand oxidation products [14]. The inner-and outer-sphere photoinduced electron transfer mechanisms have been reported for Fe 3+ complexes, that cause producing of • OH and • X (X − is the oxidizable ions or molecules present in the vicinity of the catalyst such as Cl − Br − and SCN − ), respectively [15][16][17].In the present study, nanocluster of zeolite Y was synthesized and characterized with FT-IR, XRD, thermal methods, and SEM. The zeolite was exchanged with Fe(II) solution. Then Fe(II)-o-phenanthroline/zeolite Y nano cluster (FO-ZYNC) photocatalyst was prepared. The activity of the obtained photocatalyst was evaluated by studying the photocatalytic decolorization of methyl green. The effects of catalyst dosage, methyl green concentration, pH, and temperature were studied as functions of percentage of decolorization under UV irradiation. For the sake of comparison, corresponding dark controls were also carried out.