In this study, we deposited TiO2 thin films onto borosilicate glass by ultrasonic spray pyrolysis at 350 and 450 °C. The aim of study is to determine the effect of deposition temperature on photocatalytic activity of TiO2 thin films and to investigate the performance of TiO2 thin films on photocatalytic degradation of methyl tert-butyl ether (MTBE), acetone, acetaldehyde, and heptane as functions of different operating parameters. TiO2 thin films deposited at 350 and 450 °C have a thickness value of 190 and 330 nm, respectively. All as-prepared TiO2 films possess an anatase crystalline structure. According to the X-ray photon spectroscopy (XPS) study, the TiO2 thin film deposited at 350 °C showed a higher amount of oxygen vacancies and hydroxyl groups on the film surface after UV treatment. The aged-TiO2 thin film deposited at 350 °C showed a water contact angle (WCA) value of 0° after 10 min UV irradiation, showing superhydrophilic surface behavior. The TiO2 film deposited at 350 °C exhibited the highest amount of conversion of MTBE (100%). The results also showed that TiO2 films are capable of photocatalytic degradation of MTBE (100%) and acetaldehyde (approx. 80%) in humid air conditions and high airflow rate. The visible-light-activity of TiO2 thin films was tested with 5 ppm MTBE and acetone. TiO2 thin films deposited at 350 °C with a surface area of 600 cm2 showed 60% of MTBE and 33% of acetone degradation under VIS light.