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Understanding the nature of active sites on metal oxide catalysts in the selective catalytic reduction (SCR) of NO by NH 3 (NH 3 -SCR) is a crucial prerequisite for the development of novel efficient NH 3 -SCR catalysts. In this work, two CeO 2 -based SCR catalyst systems with diverse acidic metal oxides-CeO 2 interfaces, i.e., Nb 2 O 5 -CeO 2 (Nb 2 O 5 /CeO 2 and CeO 2 /Nb 2 O 5) and WO 3 -CeO 2 (WO 3 /CeO 2 and CeO 2 /WO 3), were prepared and used to reveal the relationship between NH 3 -SCR activity and surface acidity/redox properties. In combination with the results of the NH 3 -SCR activity test and various characterizations, it was found that the NH 3 -SCR performance of Nb 2 O 5 -CeO 2 and WO 3 -CeO 2 catalysts was highly dependent on the strong interactions between the redox component (CeO 2) and acidic component (Nb 2 O 5 or WO 3), as well as the amount of paired redox-acid sites. From a quantitative perspective, an activity-surface acidity/redox property relationship was proposed. For both Nb 2 O 5 -CeO 2 and WO 3 -CeO 2 catalysts systems operated at the more concerned low-temperature range (200 °C), the NH 3 -SCR activity in low NO x conversion region (< 40%) was mainly dominated by the surface acidity of catalysts, while the NH 3 -SCR activity in high NO x conversion region (> 40%) was more determined by redox properties. [Display omitted] • Nb 2 O 5 -CeO 2 and WO 3 -CeO 2 catalysts with tuned redox-acid property were synthesized. • Paired redox-acid sites formed through strong interaction between Nb 2 O 5 /WO 3 and CeO 2. • NH 3 -SCR activity was well controlled by the paired redox-acid sites. • Surface acidity and redox property were investigated from a quantitative perspective. • A clear surface acidity/redox property-activity relationship was established. [ABSTRACT FROM AUTHOR]