In an attempt to improve surface wetting and coating characteristics, a novel technique, i.e., imposing ultrasonic vibration on the substrate, is introduced. This technique is combined with conventional ultrasonic spray coating, thus substrate vibration-assisted spray coating (SVASC), and is employed to fabricate PEDOT:PSS thin films. PEDOT:PSS is a co-polymer, commonly used as solar cell buffer layers and thin-film electrodes. Advanced surface characterization techniques, such as atomic force microscopy and confocal laser scanning microscopy are utilized. The results show that the application of the imposed vibration on the substrate results in a significant decrease in surface roughness, film thickness, and the number of defects and pin-holes. In terms of the film functionality, the electrical conductivity of the PED-OT:PSS films made using the SVASC technique shows a four-time increase, compared to those made by conventional ultrasonic spray coating. In conventional ultrasonic spray coating, increasing the number of spray passes or deposition layers usually improves the coating uniformity. For aqueous PEDOT:PSS solution and within the range of the values of the parameters investigated in this work, with imposed substrate vibration, the number of spray passes is immaterial, as far as the film uniformity is concerned. However, the application of multiple spray passes enhances the film's electrical conductivity. Our unprecedented results on the combined substrate vibration with spray coating provide a platform for low-cost fabrication of solutionprocessed thin-film solar cell devices, and a forward step toward commercialization of emerging solar cells, such as polymer and perovskite solar cells. The positive effect of using imposed substrate vibration on spray-on solar cell thin films may be deployed in other coating (e.g., spin coating) and spray coating applications as well.