This chapter describes the synthesis process to obtain zeolite Na-A from coal fly ash via fusion with NaOH followed by hydrothermal reaction. Coal fly ash is a low cost source of both silica and alumina. The molar ratio of SiO2/Al2O3 for zeolite 4A formation was achieved by the addition of sodium aluminate solution or aluminum waste from tertiary industry as aluminum sources. The effects of temperature and time at the fusion step and the hydrothermal reaction time on crystalline products were investigated. The synthesized products were studied for their purity and yield as well as were characterized by different techniques such as Xray powder diffraction (XRD), scanning electron microscopy (SEM) and cation exchange capacity (CEC), among others. Analysis of the properties of the raw materials and the products demonstrates that the by-products can be used to produce a high purity zeolite A. The optimum conditions related to the synthesis was set and the samples were pure, highly crystalline and white. The synthesized zeolites were used for both the removal of Cd (II) and Zn (II) from aqueous solution. The results showed that coal fly ash and aluminum source can be transformed into zeolite A, which is considered as value-added material with adsorption properties.Coordena????o de Aperfei??oamento de Pessoal de N??vel Superior (CAPES)