In this article, structural evolution in nickel doped zinc oxide nanostructures is reported. The ZnO nanostructures are synthesized with 1-10% of Ni doping adopting a chemical precipitation method. The undoped and doped nanostructures thus prepared, were systematically investigated employing X-ray diffraction (XRD), transmission and scanning electron microscopy (TEM/SEM), Fourier transform infrared (FTIR) and micro-Raman spectroscopy (μRS). The identification of wurtzite phase and determination of lattice parameters of Ni doped ZnO nanocrystallites is ascertained through XRD analysis. TEM/SEM images reveal the structural alteration of ZnO with variation of Ni doping concentrations. The study of vibrational modes of nanostructures at different stages of structural transformation, as performed through FTIR and Raman spectroscopy, assist in deciphering the crucial role of Ni doping concentration in gradual evolution of nickel doped ZnO structure from nanoparticles to nanorods.