- Previously we have described the deposition of vertically aligned wurtzite CdTe nanowires derived from an unusual catalytically driven growth mode. This growth mode could only proceed when the surface of the substrate was corrupted with an alcohol layer, although the role of the corruption was not fully understood. Here, we present a study detailing the remarkable role that this substrate surface alteration plays in the development of CdTe nanowires; it dramatically improves the size uniformity and largely eliminates lateral growth. These effects are demonstrated to arise from the altered surface's ability to limit Ostwald ripening of the catalytic seed material and by providing a surface unable to promote the epitaxial relationship needed to sustain a lateral growth mode. The axial growth of the CdTe nanowires is found to be exclusively driven through the direct impingement of adatoms onto the catalytic seeds leading to a self-limiting wire height associated with the sublimation of material from the sidewall facets. The work presented furthers the development of the mechanisms needed to promote high quality substrate-based vertically aligned CdTe nanowires. With our present understanding of the growth mechanism being a combination of selective area epitaxy and a catalytically driven vapour-liquid-solid growth mode, these results also raise the intriguing possibility of employing this growth mode in other material systems in an effort to produce superior nanowires.