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Chemical solution deposition was used to deposit epitaxial BaxSr(1−x)TiO3 thin films on SrTiO3 template layers on Si(001) for x = 1.0, 0.7, 0.5, 0.3, and 0.0. Effective Pockels coefficients were determined as a function of film composition both for as‐deposited films (crystallized at 600°C) and for the films after annealing at 750°C for 10 hours. Pockels response decreased monotonically with decreasing Ba content and coefficients were higher for annealed films, reaching 89 ± 3 pm/V for annealed BaTiO3. These results are contextualized with the aid of X‐ray diffraction and high‐resolution transmission microscopy, which illuminated the crystallinity and defect nature of the films. [ABSTRACT FROM AUTHOR]