Oxide materials of desired stoichiometry are challenging to make in small quantities. Nanostructured thin films of multiple oxide materials were obtained by using pulsed laser deposition and multiple independent targets consisting of Si, BaTiO3, and B. Programmable stoichiometry of nanostructured thin films was achieved by synchronizing a 248-nm krypton fluoride excimer laser at an energy of 300 mJ/pulse, a galvanometer mirror system, and the three independent target materials with a background pressure of oxygen. Island growth occurred on a per pulse basis; some 500 pulses are required to deposit 1 nm of material. The number of pulses on each target was programmed with a high degree of precision. Trends in material properties were systematically identified by varying the stoichiometry of multiple nanostructured thin films and comparing the resulting properties measured using in situ spectroscopic ellipsometry, capacitance measurements including relative permittivity and loss, and energy dispersive spectroscopy (EDS). Films were deposited ∼150 to 907 nm thickness, and in situ ellipsometry data were modeled to calculate thickness n and k. A representative atomic force microscopy measurement was also collected. EDS, ellipsometry, and capacitance measurements were all performed on each of the samples, with one sample having a calculated permittivity greater than 20,000 at 1 kHz.