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 % Y₂O₃ 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. Y³⁺ was selected based on atomistic simulations on a 4 nm zinc aluminate nanoparticle singularly doped with elements of different ionic radii: Sc³⁺, In³⁺, Y³⁺, and Nd³⁺. The segregation energies were generally proportional to ionic radii, with Y³⁺ 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/m² for Y-doped nanoparticles. Diffusion coefficients calculated from coarsening curves for undoped and doped compositions at 850 °C were 4.8 × 10^-12 cm²/s and 2.5 × 10^-12 cm²/s, respectively, indicating the coarsening inhibition induced by Y³⁺ results from a combination of a reduced driving force (surface energy) and decreased atomic mobility.