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Solid solutions of (Na,Bi)TiO3 (NBT) and SrTiO3 (ST) are materials of interest for high‐strain or high‐energy density capacitor applications. Often, they exhibit chemical heterogeneity and develop core‐shell structures during regular solid‐state synthesis with an NBT‐rich core. In this case, the NBT forms first so that the strontium needs to diffuse into the material to reach chemical homogeneity...