Precise control of Ba1−xSrxTiO3 (BST) film composition is critical for the production of high-quality BST thin films. Specifically, it is known that nonstoichiometry greatly affects the electrical properties of BST film capacitors. We are investigating the compositionmicrostructure- electrical property relationships of polycrystalline BST films produced by magnetron sputter-deposition using a single target with a Ba/Sr ratio of 50/50 and a (Ba+Sr)/Ti ratio of 1.0. It was determined that the (Ba+Sr)/Ti ratios of these BST films could be adjusted from 0.73 to 0.98 by changing the total (Ar+O2) process pressure, while the O2/Ar ratio did not strongly affect the metal ion composition. The crystalline quality as well as the measured dielectric constant, dielectric tunability, and electrical breakdown voltage of BST films have been found to be strongly dependent on the composition of the BST films, especially the (Ba+Sr)/Ti ratio. We discuss the impact of BST film composition control, through film deposition and process parameters, on the electrical properties of BST capacitors for high frequency devices.