Perovskite-structured barium strontium titanate (Ba_1-xSr_xTiO₃, x = 0.1–0.9) films have been epitaxially fabricated by using a pulsed-laser deposition technique. The third-order nonlinear optical properties were studied through a z-scan method, allowing the resolution of the nonlinear refractive and absorptive contributions to the responses. Although all the samples show almost the same value of nonlinear absorption coefficient, the extracted nonlinear refractive index of the sample of x = 0.3 is apparently larger than that of other samples. Dependency of the nonlinear optical properties on the Ba/Sr ratio is discussed in terms of the crystal phase transformation and metal-oxygen bond length of the selected materials.