This paper discusses the nucleation and growth mechanisms of ZnO nanorod thin-films and larger sized crystallites that form within the solution and on surfaces during an ultra-fast microwave heating growth process. In particular, the work focusses on the elimination of crystallites as this is necessary to improve thin-film uniformity and to prevent electrical short circuits between electrodes in device applications. High microwave power during the early stages of ZnO deposition was found to be a key factor in the formation of unwanted crystallites on substrate surfaces. Once formed, the crystallites, grow at a much faster rate than the nanorods and quickly dominate the thin-film structure. A new two-step microwave heating method was developed that eliminates the onset of crystallite formation, allowing the deposition of large-area nanorod thin-films that are free from crystallites. A dissolution-recrystallization mechanism is proposed to explain why this procedure is successful and we demonstrate the importance of the work in the fabrication of low-cost memristor devices.