The cationic interaction of binary metals in zeolite frameworks is a motivating field. Isomorphous substitution of Ti and Ce in the framework of NaY zeolite has been performed using post-synthesis treatment. Dealumination of the zeolite was performed by EDTA treatment, followed by the incorporation of Ce and Ti to decorate the metals in the zeolite framework. It was achieved in two steps based on their solubility in the corresponding solvents. The stability of the zeolite framework was studied using metal loading. It has been observed that as the amount of metals increased in the zeolite, the d spacing of the crystal lattice changed. Besides, at higher loading, certain metals are introduced into the framework, and others as exchangeable cations extra-framework in the zeolite network. The spectroscopic studies were used to characterize the modified zeolite, and the catalysts were studied for their catalytic activity in the photodegradation of 4-NP. Various parameters such as temperature, reaction time, pH, catalyst amount, and 4-NP concentration were studied to optimize the process. The synthesized catalysts show good activity for the photodegradation process. The study investigated the synergetic effect of Ce and Ti on the yield of photodegradation. The mineralization of 4-NP was confirmed by COD experiments with a removal efficiency of 68.76%. The catalyst was recoverable and maintained its catalytic activity after six runs. This finding is particularly significant as it suggests that the catalyst has the potential for industrial application and cost-effectiveness.