Root like structured Ni-doped zinc oxide [Zn(1-x)NixO (x = 0.09)] thin films were deposited on a non-conducting glass substrate by indigenously developed spray pyrolysis system at optimized substrate hotness of 573±5 K. Thus obtained Ni-doped ZnO thin films were characterized by UV-visible spectroscopy, X-ray diffraction (XRD), scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDX), Atomic Force Microscopy (AFM). XRD result revealed that Ni-doped ZnO has a polycrystalline nature with a hexagonal wurtzite structure. For pure ZnO and Ni-doped ZnO thin films, the particle sizes were 60.9 and 53.3 nm while lattice strain values were 1.56×10-3 and 1.14×10-3, respectively. The film surface showed characteristic root-like structure as observed by the SEM. It was observed that the Ni-doped ZnO thin films were grown in high density along with more extent of branching as compared to pure ZnO thin films but retained the root-like morphologies, however, the branches were more-thinner and of shorter lengths. AFM analysis showed that the surface grains of the Ni-doped samples are homogeneous with less RMS roughness values compared with the undoped ZnO samples. The photocatalytic activity of the prepared thin films was evaluated by the degradation of methyl orange (MO) dye under UV light irradiation. Pure ZnO and Ni-doped ZnO thin films took 150 min and 100 min to degrade about 60% MO dye, respectively.