Thermally stable tetragonal zirconia aerogel with a high surface area can be obtained by a novel alcohothermal route, followed by the supercritical fluid drying technique. In addition, a cheaper inorganic salt was used as raw material instead of the expensive and harmful zirconium alkoxides. The zirconia aerogel samples were characterized using X-ray diffraction, thermal analysis, N-2 adsorption measurements, diffuse reflectance infrared Fourier transform spectroscopy, and transmission electron microscopies. The results show that the resulting zirconia aerogel was composed primarily of narrowly distributed nanoparticles with loose aggregation. It is shown that the thermally stable zirconia aerogel has a high specific surface area and a well-developed textural mesoporosity with narrow pore size distribution, which is highly attractive for potential applications in heterogeneous catalysis.