Co-doped zinc oxide thin films (Zn1−x Co x O) have been deposited on c-plane sapphire substrates by dual-beam pulsed laser deposition. The films have lattice parameters similar to that of ZnO, and the lattice parameters are closely distributed. The films grew along a preferred direction, following the epitaxial relationship Zn1− x Co x O (0001)substrate (0001). Excitonic emission was suppressed at higher Co-dopant concentration in ZnO because of increase in the distortion of host lattice and defects. When more Zn is replaced by Co, more impurity levels are developed within the bandgap, and more defect are generated. Under our experimental conditions, the bandgap of the films tends to increase with increasing dopant concentration.