Using low-energy electron microscopy, we determine that self-diffusion of the Cu(001) surface is slowed by the presence of a c(2 × 2)-Pd buried surface alloy. We probe surface diffusion using Cu-adatom island-ripening measurements. On alloyed surfaces, the island decay rate decreases monotonically as the Pd concentration is increased up to ∼ 0.5 ML, where the 2 × 2 buried alloy is Pd saturated. We propose that the Pd slows island ripening by inhibiting the diffusion of surface vacancies across terraces. For dilute alloys ( < ∼ 0.2 ML Pd), this conclusion is supported by densityfunctional theory calculations which show that surface vacancies migrate more slowly owing to an attraction to isolated buried Pd atoms. The results illustrate a fundamental mechanism by which even a dilute alloy thin-film coating may act to inhibit surface-diffusion-mediated processes, such as electromigration.