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
, 550
, 650
, and 750
). 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
), while Poole–Frenkel emission plays an important role at high temperatures (above 150
) in the electrical conduction. Results suggest that the sample annealed at 650
has the most promising hydrogen-sensing performance (better current–voltage characteristics, higher sensitivity of 2.0 at 100
) among the four samples.