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[Display omitted] • Novel effect of strong acid-redox interface hinders NH 3 -SCR activity is reported. • Three Ce 2 (SO 4) 3 -CeO 2 catalysts with distinct interfaces are constructed. • NO adsorption and oxygen vacancy formation are limited after Ce 2 (SO 4) 3 addition. • Weak interface promotes NO activation and the formation of active nitrites. The occurrence of NH 3 -SCR (selective catalytic reduction of NO with NH 3) reaction on catalyst surface typically requires acid and redox sites. However, the role of acid-redox interaction on NH 3 -SCR performance is still obscure due to complex acidities and entangled acid-redox sites. Herein, three types of model Ce 2 (SO 4) 3 -CeO 2 catalysts with distinct interfaces are constructed to reveal the effect of acid-redox interaction on NH 3 -SCR performance. That is, SO 4 2-/CeO 2 -VS (vapor sulfation of ceria) with strong acid-redox interfacial contact, SO 4 2-/CeO 2 -WI (wet impregnation), and SO 4 2-/CeO 2 -SG (solid grinding) with limited interfaces. It is found the redox property is significantly disturbed as a result of the electron-withdrawing effect from the sulfate. Theoretical result unravels that the introduction of Ce 2 (SO 4) 3 retards the oxygen vacancy formation over CeO 2. Due to restricted interfaces in SO 4 2-/CeO 2 -SG, the negative influence from acid sites is greatly alleviated. Further mechanism study discloses the weakened acid-redox interaction actually changes the nature of surface NO x species, resulting in the generation of reactive species (*O-N-O* and cis -N 2 O 2 2-) and the promotion of surface reaction via Langmuir-Hinshelwood (L-H) mechanism. [ABSTRACT FROM AUTHOR]