Molybdenum oxide (MoO 3 ) thin films were prepared by pulsed-laser assisted deposition (PLD) over a wide range of growth temperature, 30–500°C. The chemical composition, crystal structure, and electrochemical properties of PLD MoO 3 thin films were investigated as a function of growth temperature. It was found that the growth temperature, and hence the thermochemical reaction during ablation, strongly influences the structural characteristics and properties of the resulting films. The compositional stability was well maintained up to a temperature on the order of 400°C, after which point the formation of compositional defects introduces structural disorder and hence the reduced phases. Electrochemical performance evaluation indicated that the PLD MoO 3 films grown at temperatures 300–400°C display charge–discharge profiles comparable to that of crystalline MoO 3 .