The optical, electrical, and structural characteristics of lanthanum-aluminum oxide thin films deposited by ultrasonic spray pyrolysis are presented. The films were deposited using a lanthanum nitrate and aluminum acetylacetonate solution in N, N-dimethylformamide on (100) Si substrates. The substrate temperature during deposition was in the 500–650°C range. The deposition activation energy was in the range of 17.4–20 kJ mol−1, depending on the relative concentration of lanthanum to aluminum in the precursor solution. The films were amorphous even at 650°C and they were given no further temperature annealing. The refractive index at 630 nm was in the range of 1.70–1.755 depending on the amount of lanthanum in the films. The electrical characteristics of the films were determined from capacitance and current versus voltage measurements of metal-oxide-semiconductor (MOS) structures incorporating them. A dielectric constant in the range of 5.2–10, and interface states density of the order of 1011-1012 eV−1 cm−2 were measured. Their electrical breakdown field was in the range of 4.5–7.6 MVcm−1 for films deposited at 500 and 550°C and a thickness under 43 nm.