We have prepared solution-processed oxide semiconductor thin-film transistors using ZnO nanoparticles with various particle shapes. Uniform, dense, thin films were produced by spin-coating ZnO nanoparticle dispersions containing either nanorods or nanospheres. The influence of annealing atmosphere on both nanoparticle-based TFT devices was investigated. XPS analysis revealed that the ZnO particles of the nanorod and nanosphere dispersions have distinct stoichiometries (i.e., molar ratios of Zn:O). The starting particles in turn predetermine the carrier concentration within the annealed ZnO films, which in turn determines whether the device is a semiconductor or metallic conductor, depending upon the annealing atmosphere. Grain structures of the channel layer also play an important role in determining the device performance of the nanoparticle derived ZnO TFTs.