The thermal stability of zinc aluminate nanoparticles is critical for their use as catalyst supports. In this study, we experimentally show that doping with 0.5 mol % Y 2 O 3 improves the stability of zinc aluminate nanoparticles. The dopant spontaneously segregates to the nanoparticle surfaces in a phenomenon correlated with excess energy reduction and the hindering of coarsening. Y 3+ was selected based on atomistic simulations on a 4 nm zinc aluminate nanoparticle singularly doped with elements of different ionic radii: Sc 3+ , In 3+ , Y 3+ , and Nd 3+ . The segregation energies were generally proportional to ionic radii, with Y 3+ showing the highest potential for surface segregation. Direct measurements of surface thermodynamics confirmed the decreasing trend in surface energy from 0.99 for undoped to 0.85 J/m 2 for Y-doped nanoparticles. Diffusion coefficients calculated from coarsening curves for undoped and doped compositions at 850 °C were 4.8 × 10 −12 cm 2 /s and 2.5 × 10 −12 cm 2 /s, respectively, indicating the coarsening inhibition induced by Y 3+ results from a combination of a reduced driving force (surface energy) and decreased atomic mobility.