Ammonia selective catalytic oxidation (NH 3 −SCO) is currently the most effective method for removing NH 3 . However, existing noble-metal catalysts still suffer from poor N 2 selectivity in NH 3 −SCO reactions. Based on Pt/ZrO 2 (P/Z), ZrO 2 support was first treated with sulfuric acid, and then Ce species were introduced to prepare Pt/Ce/ZrO 2 −S (P/C/Z-S) bifunctional catalyst. The catalytic test result showed that the P/C/Z-S catalyst possessed excellent NH 3 removal performance with a T 90 temperature of 273 °C, which was lower by 22 °C than the P/Z catalyst. The introduction of Ce species led to a significant shift of the reduction peak toward low temperatures, which greatly improved the low-temperature redox capability of the catalyst. Notably, the P/C/Z-S catalyst exhibited a much better N 2 selectivity (>90%) in a wide temperature range (320−450 °C). The introduction of S species significantly enhanced the number of acid sites (especially Brønsted acid sites) at the catalyst surface. It promoted the NH 3 adsorption capacity of the P/C/Z-S catalyst obviously. On the other hand, the introduced Ce species provided more redox active sites, which would accelerate the activation and reaction of adsorbed NH 3 species. The sulfuric acid treatment of the ZrO 2 support and the introduction of Ce species resulted in abundant adsorbed oxygen at the catalyst surface. It was beneficial to dihydrogen adsorbed NH 3 to amide (−NH 2 ) species, which subsequently underwent ammonia selective catalytic reduction (NH 3 −SCR) reactions with NO over Ce sites. This study can enrich the insights into the design of efficient NH 3 −SCO catalysts by tuning acidic and redox active sites.