Atomic layer deposition (ALD) is a very promising deposition technique for ZnO thin films. However, there have been very few reports on ZnO grown by ALD. Effects of substrate temperature in both ALD and post annealing on the microstructure and PL properties of ZnO thin films were investigated using X-ray diffraction, photoluminescence, and scanning electron microscopy. The temperature window of ALD is found to be between [Math Processing Error] . The growth rate of ZnO thin film increases as the substrate temperature increases in the temperature range except the temperature window. The crystal quality depends most strongly on the substrate temperature among all the growth parameters of ALD. The crystallinity of the film is improved by increasing the growth thine per ALD cycle or doing post-annealing treatment. The grain size of the film tends to increase and the grain shape tends to change from a worm-like longish shape to a round one as the annealing temperature increases from [Math Processing Error]