Perovskite-structured LaxSryMnO3 thin-films have been deposited onto LaAlO3 substrates via liquid delivery chemical vapor deposition (LD-CVD) using metal(β-diketonato) precursors, M(thd)x [where M= Ca, Sr, La and Mn, thd = 2,2,6,6-tetramethyl-3,5-heptanedionato and x = 2–3]. Thin films were deposited at temperatures between 500 and 700 °C and subsequently annealed at 1000 °C under O2. These films possess stoichiometries that are: i) vastly different from the La0.67Sr0.33MnO3 compositions commonly reported in the literature and ii) display high temperature, low field responses that may be technologically important. Resistance versus temperature measurements revealed a metal to semiconductor transition at room temperature and above. Hall measurements on a film of La0.35Sr0.24MnO3 displayed a magnetoresistive response (MR) of -10% at 57 °C in a fixed magnetic field of 780 Oe. Based upon our research, the observed film properties are directly related to the deposited film stoichiometry and the best results were observed at Sr / La ratios between 0.30 and 1.0 for A-site deficient LaxSryMnO3 thin-films after thermal annealing.