The removal characteristics of NH3 based on chemical-looping combustion (CLC), in which NH3 was used as a fuel, were studied. Results indicated that in the reduction reaction between oxidative oxygen carriers (OCs) and NH3, the oxidative OCs were converted to reductive OCs, and at the same time, NH3 was converted to N-2 and H2O. Then, the reductive OCs were regenerated to the oxidative OCs with air in the subsequent oxidation reaction. As such, NH3 removal with high N-2 selectivity was achieved based on CLC. Compared to MnO2/Al2O3 and Fe2O3/Al2O3, CuO/Al2O3 exhibited the highest NH3 removal activity, and an NH3 removal rate of 90% with a N-2 selectivity of 99% was achieved at 250 degrees C. Among three Cu-based OCs, i.e., CuO/Al2O3, CuO/TiO2, and CuO/SiO2, CuO/Al2O3 using gamma-Al2O3 as inert support performed the highest NH3 removal activity and N-2 selectivity. Moreover, the required temperature for the complete regeneration of the reductive CuO/Al2O3 with air was as low as 200 degrees C. However, due to its overly high oxidizability, O-2 that existed in the waste gas deteriorated the N-2 selectivity. On the basis of these findings, a new process for NH3 deep removal with high N-2 selectivity based on CLC coupled with adsorption enrichment was proposed.