Titania-modified zirconias with different Ti/Zr ratios were synthesized via thermal treatment of zirconium (IV) tetra-n-propoxide and titanium (IV) tetra-iso-propoxide in 1,4-butanediol at 300 °C. The obtained products were spherical particles composed of nanocrystals with the tetragonal ZrO2 structure. The products had large specific surface areas, large pore volumes, and relatively narrow pore size distributions in the mesopore region. After calcination at high temperatures, the obtained TiO2-modified ZrO2 samples preserved large surface areas and pore structure. Having these superior thermal stability and pore structure, the obtained TiO2-modified ZrO2 particles are expected to show high performance as catalytic materials.