Organic semiconductor nanoparticles are expected to be used in organic optical and electronic devices due to their unique optical and electrical properties. However, no method has been reported for the preparation of high-quality organic nanoparticle films without remaining additives and being capable of dealing with binary nanoparticle blends. We developed a simple approach to fabricate high-quality organic semiconductor nanoparticle films from their aqueous solutions by solvent-evaporation-induced self-assembly. Only volatile solvents are employed in the nanoparticle solutions, so the self-assembled nanoparticle films are free of additives. Moreover, this method is also suitable for fabricating thin films containing binary nanoparticles. Therefore, it paves the way for potential applications of organic semiconductor nanoparticles in nanoscale optical and electronic devices.