The catalytic activities for N2O decomposition and selective reduction with methane were studied on Fe-MCM-41 prepared by direct hydrothermal synthesis (DHT) and template ion exchange (TIE) methods. Fe-MCM-41-DHT showed higher activity than those prepared by TIE and impregnation methods. The high activity of Fe-MCM-41-DHT is caused by the formation of highly isolated and tetrahedrally coordinated iron-oxo species.