We successfully deposited LiAlO2 films on Si substrates at 400–600 °C by single source chemical vapor deposition using a heterometallic compound, Li(O'Pr)2Al(CH3)2, which contains Li, Al, and O at the same 1:1:2 ratio as LiAlO2. Li(O'Pr)2Al(CH3)2 is sufficiently volatile to be vapor-transported at 50 °C. Elastic recoil detection and Rutherford backscattering spectroscopy analyses of a deposited film indicate that the film is stoichiometric (Li:Al:O = 1.0:1.0:2.0) and contains a few atomic percent hydrogen (5 %) and carbon (2 %). Depth profile analysis of X-ray photoelectron spectroscopy also confirms the 1:1 ratio of metal contents in the films. As-deposited films were amorphous, however, crystallized to β- or γ-LiA1O2 after annealing at 950 °C.