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In this paper, by using a metal-insulator-semiconductor Schottky-diode structure, we examined the electrical and hydrogen-sensing properties of radio frequency sputtered LaTiON thin films that had been annealed at four different temperatures (450°C, 550 °C, 650°C, and 750°C). Characterization of their morphological surface indicates that their average surface roughness decreases from 0.108 to 0.090 nm with increasing annealing temperature. X-ray diffraction shows the growths of La and Ti are in the 1 0 0 direction, i.e., in parallel to the Si substrate. Analysis of measured electrical characteristics indicates that thermionic emission is the dominant mechanism at low temperatures (from RT to 150°C), while Poole-Frenkel emission plays an important role at high temperatures (above 150 °C) in the electrical conduction. Results suggest that the sample annealed at 650°C has the most promising hydrogen-sensing performance (better current-voltage characteristics, higher sensitivity of 2.0 at 100°C) among the four samples.