A novel spindle-like zinc oxide (ZnO) nanocrystalline thin film was successfully fabricated on Ni thin film layer by ultrahigh-vacuum dc magnetron sputtering. Then the as-grown films were annealed in air at various temperatures from 673 to 1073 K, the corresponding structural features and surface morphology were studied by X-ray diffraction (XRD) and field emission scanning electronic microscopy (FE-SEM). The results reveal that the dominant direction of grains movement changed from perpendicular to parallel to the film interfaces. A correlation of the band gap and photoluminescence (PL) properties of nanocrystalline ZnO films with particle size morphologies and strain was discussed. Especially, PL emission in UV range, which is due to near band edge emission is more intense in comparison with the green band emission (due to defect state) was observed in all samples, indicating a good optical quality of the deposited films.