Ultrasonic spray pyrolysis is a deposition technique that enables a fine mist of the precursor solution in order to deposit higher-density thin films. This characteristic makes of great potential the use of ultrasonically spray-deposited semiconductors films for lowcost, transparent, flexible and large-area applications. In this chapter, low-temperature deposition and characterization of ultrasonically spray-deposited zinc oxide (ZnO) films are presented. The ZnO films deposited by ultrasonic spray pyrolysis at 200°C were characterized by optical transmittance, photoluminescence spectroscopy, X-ray diffraction and Fourier transform infrared spectroscopy. The study of low-temperature annealing of ZnO films is also presented. Moreover, the characterization of aluminum-doped ZnO films deposited by ultrasonic spray pyrolysis at 200°C is presented. Finally, applications of these ultrasonic spray-deposited films in electronic devices are presented.