The production mechanism of OH radicals in a pulsed DC plasma jet is studied by a two-dimensional (2-D) plasma jet model and a one-dimensional (1-D) discharge model. For the plasma jet in the open air, electron-impact dissociation of H2O, electron neutralization of H2O+, as well as dissociation of H2O by O(1D) are found to be the main reactions to generate the OH species. The contribution of the dissociation of H2O by electron is more than the others. The additions of N2, O2, air, and H2O into the working gas increase the OH density outside the tube slightly, which is attributed to more electrons produced by Penning ionization. On the other hand, the additions of O2 and H2O into the working gas increase the OH density inside the tube substantially, which is attributed to the increased O (1D) and H2O concentration, respectively. The gas flow will transport high density OH out of the tube during pulse off period. It is also shown that the plasma chemistry and reactivity can be effectively controlled by the pulse numbers. These results are supported by the laser induced fluorescence measurements and are relevant to several applications of atmospheric-pressure plasmas in health care, medicine, and materials processing.