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Zinc oxide (ZnO) nanomaterials are used in various health-related applications, from antimicrobial textiles to wound dressing composites and from sunscreens to antimicrobial packaging. Purity, surface defects, size, and morphology of the nanoparticles are the main factors that influence the antimicrobial properties. In this study, we are comparing the properties of the ZnO nanoparticles obtained by solvolysis using a series of alcohols: primary from methanol to 1-hexanol, secondary (2-propanol and 2-butanol), and tertiary (tert-butanol). While the synthesis of ZnO nanoparticles is successfully accomplished in all primary alcohols, the use of secondary or tertiary alcohols does not lead to ZnO as final product, underlining the importance of the used solvent. The shape of the obtained nanoparticles depends on the alcohol used, from quasi-spherical to rods, and consequently, different properties are reported, including photocatalytic and antimicrobial activities. In the photocatalytic study, the ZnO obtained in 1-butanol exhibited the best performance against methylene blue (MB) dye solution, attaining a degradation efficiency of 98.24%. The comparative study among a series of usual model dyes revealed that triarylmethane dyes are less susceptible to photo-degradation. The obtained ZnO nanoparticles present a strong antimicrobial activity on a broad range of microorganisms (bacterial and fungal strains), the size and shape being the important factors. This permits further tailoring for use in medical applications. [ABSTRACT FROM AUTHOR]