The possibilities for fabricating solid solutions of (Ba1−x,Srx)TiO3 (x≤0.5,1.0) by crystallization of amorphous films and for improving their dielectric properties by adjusting the Sr content were investigated. Thin amorphous films were prepared from powder targets consisting of mixtures of BaTiO3 and SrTiO3 by sputtering with a neutralized Ar-ion beam. The amorphous films crystallized into (Ba1−x, Srx)TiO3 solid solutions with a cubic perovskite-type structure after annealing in air at 923 K for more than 1 h. The Debye-type dielectric relaxation was observed for the amorphous films, whereas the crystallized films showed paraelectric behavior. The relative dielectric constants were of the order of 20 for the amorphous samples, but increased greatly after crystallization to about 60–200, depending on the composition; a larger increase in the dielectric constant was observed in the higher Sr content films, in the range x≤0.5, which could be correlated with an increase in the grain size of the crystallites. The crystallization processes responsible for the difference in the grain size are discussed based on the microstructural observations.