Thickness-dependent electrical, structural, and optical properties of zinc oxide (ZnO) thin films on polyethylene terephthalate (PET) substrates have been investigated in the very thin thickness range of 20 to 120 nm. In this thickness range, the electrical resistance of ZnO film increased with an increase in film thickness. This unusual transition behavior was explained in terms of structural evolution from Zn-phase-incorporating non-crystalline ZnO to hexagonal-structured ZnO. A critical thickness for the full development of hexagonal ZnO crystal was estimated at approximately 80 nm in this study. ZnO thin films on PET substrates exhibit a high optical transmittance of >70% and good endurance to bending cycles over the measured thickness range. The results of this study indicate that a trade-off should be sought between structural, electrical, optical, and mechanical properties for practical applications of very thin ZnO films on organic substrates. (C) 2016 Elsevier B.V. All rights reserved.