The sol-gel technique is well known and widely used for manufacturing coatings. An aerosol-gel method is a modification of the classic sol-gel process. Preparation of coatings by this technique involves the formation of an aerosol and its deposition on the coated surfaces, where the aerosol droplets merge into a continuous layer. In this work, an aerosol-gel routine, enhanced with a low-temperature plasma discharge, was used to produce zirconia coatings on different substrates. Low-temperature plasma was used for preactivation of substrate surfaces prior to the sol deposition, and for treatment of deposited layers. The obtained coatings were characterized using optical, electron (SEM), and atomic force (AFM) microscopes, a contact-angle device, a scratch tester, a grazingincidence X-ray diffractometer (GIXRD), and an infrared spectrometer (FTIR). The results showed a significant influence of substrate plasma pretreatment on the formation and morphology of zirconia thin films. A noticeable effect of low-temperature plasma treatment on the structure and properties of the obtained coatings was also presented. These results allow possible applications of this method for the preparation of zirconia coatings on temperature-sensitive substrates to be predicted.