Ceramic compositions of barium strontium titanium oxide (BSTO) have been formulated for applications as pyroelectric sensor materials. The material has been fabricated in tape-cast and thin film forms. In general, the materials demonstrated high pyroelectric coefficients (p) accompanied with low dielectric constant and low dissipation factor. The compositions of the tape-cast and thin film specimens examined in this paper include a well-known commercially adopted Ba0.64Sr0.36TiO3 as well as a composition suggested in the literature, and a patented composition with the addition of MgO to BSTO is investigated. Doping BSTO with MgO has been shown to reduce the dielectric constant and loss tangent (over a very wide frequency range from 100 Hz-10 GHz) of the material and thereby increase the pyroelectric figure of merit. This article will discuss the processing, material characterization, pyroelectric coefficient, and pyroelectric figure-of-merit of the above mentioned BSTO compositions.