Catalytic properties of supported gallium oxides have been examined for the selective reduction of NO by CH4 in excess oxygen. The activity was greatly affected by the support; Ga2O3/Al2O3 (Al2O3 supported Ga2O3) and Ga2O3-Al2O3 mixed oxide exhibited high activity and selectivity as comparable to Ga-ZSM-5, while unsupported Ga2O3 and the other supported Ga2O3 were ineffective. For Ga2O3/Al2O3, the activity changed with Ga2O3 content, and was highest at about 30 wt% Ga2O3, which corresponds to a theoretical monolayer coverage. Gallium oxide highly dispersed on Al2O3 is considered to be responsible for the high activity and selectivity. The reaction characteristics of Ga2O3/Al2O3 were studied and compared with Ga-ZSM-5 and Co-ZSM-5. Ga2O3/Al2O3 exhibited the highest activity and selectivity at high temperature. In addition, Ga2O3/Al2O3 showed higher tolerance against water than Ga-ZSM-5. C3H8 and C3H6 were also evaluated as reducing agents, and Ga2O3/Al2O3 showed higher activity than Ga-ZSM-5 above 723 K achieving almost complete reduction of NO to N-2.