The hydrophobic rutile titania aerogels were successfully prepared by nonalkoxide ambient pressure drying through a modification process. The resulted materials were characterized by x-ray diffraction, scanning electronic microscope, transmission electron microscope, contact angle analyzer, Brunauer–Emmett–Teller specific surface area, and ultraviolet (UV)–visible diffuse reflection spectrum. The experimental results demonstrated that the as-prepared samples nanoparticles with rutile crystalline structure were uniformly distributed. The UV-resistant hydrophobic samples having high surface area were used as photocatalysts for dye degradation reaction.