Atomically dispersed metal catalysts often exhibit superior performance compared to that of nanoparticle catalysts in many catalysis processes. However, these so-called "singleatom" catalysts have a consistently low loading density on the support surface and easily aggregate at high temperatures, hindering their practical application. Herein, we demonstrate a facile surface engineering protocol using molecule−surface charge transfer adducts to fabricate highly stable noble metal catalysts with atomic dispersion, using a Pt/CeO 2 catalyst as an example. The key of this approach is the generation of an adequate amount of Ce 3+ defective sites on the porous CeO 2 surface through the adsorption of reductive ascorbic acid molecules and a subsequent surface charge transfer process. Subsequently, noble metal Pt atoms can be well-dispersedly anchored onto the generated Ce 3+ sites of porous CeO 2 nanorods with a loading density of up to 1.0 wt %. The as-prepared highly dispersed Pt/CeO 2 catalyst showed outstanding catalytic activity at near room temperature toward CO oxidation, with excellent stability over several days, which is far superior to the traditional impregnation-prepared catalysts, the activity (complete conversion at 90 °C) of which is severely decayed within a couple of hours. The proposed synthetic route is simple yet versatile and can therefore be potentially applied to fabricate other supported noble metal catalysts with atomic dispersion.