A series of nanostructured ferroelectric thin films of barium strontium titanate were fabricated using a pulsed laser deposition system with real-time in situ process control. Pulsed laser deposition parameters were controlled during the growth of nanostructured thin films for use in the development of high frequency tunable microwave devices. The thin films were all grown at the same substrate temperature and laser beam energy density, but the chamber oxygen partial pressure (COPP) was varied systematically from 19 mTorr through 1000 Torr. Structural and electromagnetic characterization was performed using atomic force microscopy and evanescent microwave microscopy, respectively. Atomic force microscopy showed a linear increase in grain size with increases in the ambient oxygen pressure from 38 to 150 mTorr and from 300 mTorr to 1000 Torr. The correlation of the microwave properties with the epitaxial film microstructure can be attributed to stresses and polarizability in the film. Microwave characterization showed that a COPP of 75 mTorr yielded the most desirable film in terms of tunability and loss tangent over a wide frequency range.