Increasing gas turbine operating temperatures are driving the development of novel coatings for niche applications. One such application is as an anchor phase material for use in the high-pressure turbine stage, for which NiAlTa alloys are a promising candidate. Extended exposure to the high temperatures of this environment can cause interdiffusion of elements between the coating and the underlying blade material. In this study, NiAlTa/CMSX-4 diffusion couples were investigated experimentally and computationally. The couples initially contained two two-phase regions (γ + γ′) and (β + τ1). After heat treatment at 1100 °C, interdiffusion had caused the τ1 Laves phase in the coating to transform to the τ2 Heusler phase, and TCP precipitation was observed in the CMSX-4. A CALPHAD-based model, using Thermo-Calc and DICTRA, developed for this system was able to predict the concentration profiles across the diffusion couple at 1000 °C, with the presence of the predicted phases in the interdiffusion zone verified by x-ray diffraction. However, due to the limited diffusion data for intermetallic phases available in the kinetic database, the model predictions were poor at higher temperatures. In order for the development of intermetallic coatings to be aided by CALPHAD-based simulations, more kinetic data is needed for intermetallic phases than is available at present.