In summary, we have reported an alternative method for synthesizing ZnO nanostructures with excellent crystallinity. With In inclusion in the growth process, the morphology of products can be changed from nanopins to nanowires. In addition, we demonstrate that the main effects of In inclusion are to decrease the velocity of crystallization, improve crystalline quality, and reduce defect concentration. The luminescence intensity can be enhanced by more than one order of magnitude. Our result therefore provides an excellent route to obtain high quality nanomaterials of ZnO for optoelectronic applications.