In this study, NaA zeolite was successfully synthesized from coal gangue with high contents of iron and quartz as the main raw material. The results show that most iron ions can be removed from coal gangue after calcination at 700 °C for 2 h, leaching in hydrochloric acid with a mass fraction of 20% for 7 h and a liquid-solid ratio of 3.5:1. When m (acid leached residue of calcined gangue):m (Na2CO3) = 1.1 and melting at 750 °C for 2 h, the quartz and other aluminosilicates turn into nepheline, which dissolve in water. Finally, the optimum conditions of synthesis NaA zeolite are as follows: n(SiO2)/n(Al2O3) = 2.0, n(Na2O)/n(SiO2) = 2.1, n(H2O)/n(Na2O) = 55, aging at 60 °C for 2 h, and crystallization at 94 °C for 4 h. This shows that the high iron and quartz contents coal gangue can be used for the synthesis of NaA zeolite.