The cationic interaction of binary metals in zeolite frameworks is a motivating feld. The Isomorphous substitution of Ti and Ce in the framework of NaY zeolite has been achieved through post-synthesis treatment. Dealumination of the zeolite was accomplished by EDTA treatment, followed by the incorporation of three distinct ratios of Ce [(4.5–9)× 10−4 M] and Ti [(1.7–5.1)× 10−5 M] for decoration on the zeolite framework. This process was carried out in two steps based on their solubility in the corresponding solvents. The stability of the zeolite framework was assessed using metal loading. It was observed that as the amount of metals in the zeolite increased, the d spacing of the crystal lattice changed. Besides, certain metals were introduced at higher loading into the framework, while others acted as exchangeable cations in the extra-framework of the zeolite network. Spectroscopic studies were conducted to characterize the modifed zeolite, and the catalysts were performed for their catalytic activity in the photodegradation of 4-NP. The optimum conditions were obtained with various parameters as: 0.01 g catalyst, 20 μL H2O2, 4-NP concentration: 3× 10−4 M, pH=5.5, and t=120 min. In addition, the study of optimum conditions in the pH=5 and isoelectric point=5.5 indicated that the removal of 4-NP was achieved using both the absorption and photodegradation processes. The synthesized catalysts show good activity in the photodegradation process. This study also investigated the synergistic efect of Ce and Ti on photodegradation efciency. The mineralization of 4-NP was confrmed by COD experiments, resulting in an efciency of 68.76%. The catalyst was recoverable and maintained its catalytic activity after six runs. The kinetic of the reaction was obtained based on Hinshelwood’s equation which was pseudo-frst-order. In addition, the band gap of the catalyst was also calculated. This fnding is particularly important because it indicates that the catalyst has the potential for industrial application and is cost-efectiveness.