Zinc oxide films derived from drop-coating solutions of zinc acetate in ethanol followed by chemical bath deposition were examined for their suitability as buffer layers for high temperature vapor phase deposition of large area, aligned, zinc oxide nanorod arrays. An X-ray photoelectron spectroscopy analysis of substrates drop coated with zinc acetate solutions clarifies the chemistry of the deposition mechanism of the initial acetate-derived ZnO seeds. Scanning electron microscopy, atomic force microscopy, and white light profilometry studies show that while zinc acetate-derived buffer layers are suitable for chemical bath deposition of aligned zinc oxide nanorod arrays, during high temperature vapor phase depositions these buffer layers undergo substantial changes leading to a loss of nanorod alignment and poor substrate coverage. We present a method to deposit aligned zinc oxide nanorod arrays uniformly over large area substrates, which combines zinc acetate drop coating, chemical bath deposition of buffer layers, and vapor phase transport deposition of nanorods. © 2010 American Chemical Society.