Zinc oxide (ZnO) is well known to the electronic industry as a piezoelectric material. Recent research from this laboratory also indicates the potential of ZnO as a tribological material. The current work describes the evolution of microstructure with deposition parameters in pulsed laser deposited ZnO thin films, specifically targeted for friction and wear applications. Films were characterized by high resolution scanning electron microscopy (SEM), transmission electron microscopy (TEM), and X-ray diffraction (XRD). Friction and wear measurements were made using a ball-on-disk tribometer. Films were grown in vacuum (V) as well as in 5 mTorr of oxygen (O-2), while the substrates were kept at room temperature (RT). The RT/V ZnO films have (002) columnar texture with an average column width of 20 nm. The RT/O-2 films also are nanoclumnar with (002) texture, but each column is a mosaic of low-angle boundaries. Deformation mechanisms associated with nanocrystalline grain structure were analyzed with particular reference to sliding contact. Mechanisms to provide the observed low friction of RT/O-2 films (mu = 0.15-0.20) have been activated by its mosaic structure.