Thin films of yttria-stabilized zirconia (YSZ) nanoparticles were prepared using a low-temperature deposition and crystallization process involving successive ionic layer adsorption and reaction (SILAR) or SILAR-Air spray Plus (SILAR-A+) methods, coupled with hydrothermal (175 °C) and furnace (500 °C) post-annealing. The annealed YSZ films resulted in crystalline products, and their phases of monoclinic, tetragonal, and cubic were categorized through X-ray diffraction analysis. The morphologies of the as-prepared films, fabricated by SILAR and SILAR-A+ processes, including hydrothermal dehydration and annealing, were characterized by the degree of surface cracking using scanning electron microscopy images. Additionally, the thicknesses of the YSZ thin films were compared by removing diffusion layers such as spectator anions and water accumulated during the air spray plus process. Crack-free YSZ thin films were successfully fabricated on glass substrates using the SILAR-A+ method, followed by hydrothermal and furnace annealing, making them suitable for application in solid oxide fuel cells.