Thin films of titanium dioxide (TiO2) nanocrystals, widely acknowledged for their unique physical-chemical properties and functionalities, are used in disparate technological fields, including photovoltaics, sensing, environmental remediation and energy storage. In this paper, the preparation of thin films consisting of anatase-phase TiO2 nanorods deposited using the matrix-assisted pulsed laser evaporation (MAPLE) technique and their characterization in terms of morphology, elemental composition and wettability are presented and discussed. Particular attention is paid to the effects of the laser fluence, varied over a broad range (F = 25, 50, 100 mJ/cm2), and to the role of the capping surfactants bound to the surface of the nanorod precursors. Whereas increasing fluence favored a partial removal of the surface-bound surfactants, a post-growth UV-light-driven photocatalytic treatment of the films was found to be necessary to reduce the incorporated fraction of organics to a further substantial extent. It was noteworthy that, under our experimental conditions, the distinctive surface patterns and roughness that commonly degrade the morphology of films deposited using the MAPLE technique were not observable. This previously unreported experimental evidence was rationalized on the basis of the interaction dynamics between solvent/solute droplets ejected from the laser-irradiated target and the rough surfaces of the growing film.