The PDF file includes:

• Supplementary Text
• Fig. S1. Formation of the bimetallic domain structures.
• Fig. S2. Oxygen-induced surface restructuring.
• Fig. S3. Statistical analysis plots for NiO_{1− x} clusters.
• Fig. S4. Direct observation of the Pt₃Ni(111) after CO/O₂ gas evacuation.
• Fig. S5. AP-XPS analysis at 100 mtorr of O₂.
• Fig. S6. Tracking the mass profiles at room temperature.
• Fig. S7. AP-XPS analysis in mixed CO/O₂ gas at elevated temperature.
• Fig. S8. Arrhenius plots for catalytic activity measurements.
• Fig. S9. Model structures of the interfacial Pt-NiO_{1− x} and NiO/Pt₃Ni.
• Fig. S10. Energy profile for CO oxidation on the Pt(111).
• Fig. S11. Activation barriers for the CO oxidation reaction (CO* + O* → CO₂) for different O* configurations on the model surfaces.
• Fig. S12. Energy profile for O₂ dissociation on the Pt(111) surface and on the interfacial Pt-NiO_{1− x} nanostructure.
• Legend for movie S1

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Other Supplementary Material for this manuscript includes the following:

• Movie S1 (.avi format). Time-lapse AP-STM movie on the Pt₃Ni(111) surface under mixed CO/O₂ (1:5 ratio) gas at 300 K.