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Abstract Oxide supports with well‐defined shapes enable investigations on the effects of surface structure on metal–support interactions and correlations to catalytic activity and selectivity. Here, a modified atomic layer deposition technique was developed to achieve ultra‐low loadings (8–16 ppm) of Pt on shaped ceria nanocrystals. Using octahedra and cubes, which expose exclusively (111) and (100) surfaces, respectively, the effect of CeO₂surface facet on Pt‐CeO₂interactions under reducing conditions was revealed. Strong electronic interactions result in electron‐deficient Pt species on CeO₂(111) after reduction, which increased the stability of the atomically dispersed Pt. This afforded significantly higher NMR signal enhancement in parahydrogen‐induced polarization experiments compared with the electron‐rich platinum on CeO₂(100), and a factor of two higher pairwise selectivity (6.1 %) in the hydrogenation of propene than any previously reported monometallic heterogeneous Pt catalyst.