We present the first structure determination by surface x-ray diffraction during the restructuring of a model catalyst under reaction conditions, i.e., at high pressure and high temperature, and correlate the restructuring with a change in catalytic activity. We have analyzed the Pt(110) surface during CO oxidation at pressures up to 0.5 bar and temperatures up to 625 K. Depending on the O 2 =CO pressure ratio, we find three well-defined structures: namely, (i) the bulk-terminated Pt(110) surface, (ii) a thin, commensurate oxide, and (iii) a thin, incommensurate oxide. The commensurate oxide only appears under reaction conditions, i.e., when both O 2 and CO are present and at sufficiently high temperatures. Density functional theory calculations indicate that the commensurate oxide is stabilized by carbonate ions (CO 2ÿ 3 ). Both oxides have a substantially higher catalytic activity than the bulk-terminated Pt surface.