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Over the last decades, the spin-coating (SC) technique has been widely used to prepare thin films of various materials in the liquid phase on arbitrary substrates. The technique simply relies on the centrifugal force to spread a coating solution radially outward over the substrate. This mechanism works fairly well for solutions with low surface tension to form thin films of reasonable junctions on smooth substrates. Here, we present a modified SC technique, namely, ultrasonic-assisted spin-coating (UASC), to form thin films of coating solution having high surface tension on rough substrates with excellent junctions. The UASC technique couples SC with an external ultrasonic wave generator to provide external perturbation to locally break down big drops of the coating material into smaller droplets via Rayleigh instability. Because of their lower mass, these tiny droplets gain low momenta and move slowly both in radial and azimuthal directions, giving them an enough time to effectively permeate within pores, thereby yielding excellent junctions. Furthermore, we also investigated the effect of junction improvement on conventional and inverted bulk heterojunction organic solar cells. Intriguingly, the organic solar cells fabricated by the UASC method showed an improved efficiency compared to typical SC owing to efficient charge transfer across the junction. These results clearly imply that UASC is a simple and powerful technique which can significantly enhance the device performance by improving the junction. Moreover, we believe that UASC can be more effective for the preparation of devices composed of multilayers of different materials having complicated nanostructures.