Raman spectrum is performed to study the phonon modes of Ni-doped ZnO powders. The phonon mode of undoped ZnO and two additional modes (AMs) have been observed in the Raman spectra of doped swatch. The observation of E2(h) phonon mode in the samples indicates that the doped ZnO powders still keep the hexagonal structure. The AM at 652 cm-1 is ascribed as local vibrational mode due to the host defects. In order to identify the origin of the AM at 544 cm-1, Raman spectrums of the Ni-, Co-, and Mn-doped ZnO powders have been carried out respectively. The results show that the AM at 544 cm-1 is related to Ni impurity. Origins of other phonon modes in the spectra are discussed as well. The multi-LO phonons scattering observed by an exciting source of 325 nm on Ni-doped ZnO powders is reported.