The metal-support interactionplays a crucialrole in determiningthe catalytic activity of supported metal catalysts. Changing thefacet of the support is a promising strategy for catalytic controlvia constructing a well-defined metal-support nanostructure.Herein, we developed cubic and octahedral Cu2O supportswith (100) and (111) facets terminated, respectively, and Pt nanoparticles(NPs) were introduced. The in situ characterizationsrevealed the facet-dependent encapsulation of the Pt NPs by a CuOlayer due to the oxidation of the Cu2O support during theCO oxidation reaction. The CuO layer on Pt at cubic Cu2O (Pt/c-Cu2O) significantly enhanced catalytic performance,while the thicker CuO layer on Pt at octahedral Cu2O suppressedCO conversion. The formation of a thin CuO layer is attributed tothe dominant Pt-O-Cu bond at the Pt/c-Cu2O interface, which suppresses the adsorption of oxygen molecules.This investigation provides insight into designing high-performancecatalysts via engineering the interface interaction.