ZnO plasma produced by third harmonic 355 nm of Nd:YAG laser at various ambient pressures of oxygen was used for depositing quality nanocrystalline ZnO thin films. Time and space resolved optical emission spectroscopy is used to correlate the plasma properties with that of deposited thin films. The deposited films showed particle size of 8 and 84 nm at ambient oxygen pressure of 100 and 900 mTorr, respectively. Third harmonic generation observed in ZnO thin films deposited under 100 mTorr of ambient oxygen is reported. © 2005 Elsevier B.V. All rights reserved.