A novel photocatalyst, FeTPyPY, was prepared by immobilizing water-soluble tetra (4-pyridyl) phenyl iron-porphyrin (FeTPyP) on NaY zeolite to degrade microcystin-LR (MC-LR), one of the most toxic microcystins (MCs). UV-Vis analysis, UV-Vis diffuse reflectance spectroscopy, infrared spectroscopy, cyclic voltammetry and transmission electron microscopy were employed to characterize immobilized FeTPyPY. Under visible light (λ ≥ 420 nm), MC-LR was degraded utilizing immobilized FeTPyPY by activating molecular oxygen. The results showed that 85% of MC-LR was efficiently degraded by FeTPyPY with loading amount 100:1 (mNaY:mFeTPyP) after 300 min of visible light illumination. Moreover, FeTPyPY was stable in the degradation system with pH 7.0. The degradation mechanism was evaluated using electron spin resonance, and the results demonstrated that highly reactive oxygen species (•OH radical) were generated in the system to degrade MC-LR. Therefore, immobilized FeTPyPY was available to break down the toxic groups within MC-LR by utilizing environmental •OH radical under circumneutral condition.