In this study, CeZr0.5TiaOx (with a = 0, 1, 2, 5, 10) catalysts were prepared by a stepwise precipitation approach for the selective catalytic reduction of NOx with NH3. When Ti was added, all of the Ce-Zr-Ti oxide catalysts showed much better catalytic performances than the CeZr0.5Ox. Particularly, the CeZr0.5Ti2Ox catalyst showed excellent activity for broad temperature range under high space velocity condition. Through the control of pH value and precipitation time during preparation, the function of the CeZr0.5Ti2Ox catalyst could be controlled and the structure with highly dispersed CeO2 (with redox functions) on the surface of ZrO2-TiO2 (with acidic functions) could be obtained. Characterizations revealed that the superior catalytic performance of the catalyst is associated with its outstanding redox properties and adsorption/activation functions for the reactants.