A zeolite material (ZCH) was synthesized from coal fly ash in an HD thermal power plant using a fusion/hydrothermal method. ZCH with high crystallinity could be synthesized at the NaOH/CFA ratio of 0.9. Ion-exchanged ZCH adsorbents for ammonia removal were prepared by ion-exchanging various cation (Cu2+, Co2+, Fe3+, and Mn2+) on the ZCH. They were used to evaluate the ammonia adsorption breakthrough curves and adsorption capacities. The ammonia adsorption capacities of the ZCH and ion-exchanged ZCHs were high in the order of Mn-ZCH > Cu-ZCH ≅ Co-ZCH > Fe-ZCH > ZCH according to NH3-TPD measurements. Mn-ZCH ion-exchanged with Mn has more Brønsted acid sites than other adsorbents. The ion-exchanged Cu2+, Co2+, Fe3+, or Mn2+ ions uniformly distributed on the surface or in the pores of the ZCH, and the number of acidic sites increased on the alumina sites to form the crystal structure of zeolite material. Therefore, when the ion-exchanged ZCH was used, the adsorption capacity for ammonia gas increased.