This study has established a three-solvent methodology for separating nanomaterials, such as monometallic nanoparticles, miscible and immiscible nanoalloys. After systematically investigating the separation methods in two-solvent and three-solvent systems, a three-solvent theoretical model has been proposed to thoroughly reveal the centrifugation mechanism of colloidal particles. PVP plays an important role in the formation of emulsion droplets as the key factor for separation. Based on the three-solvent model, a novel solvent system has been discovered, with low-toxicity solvents and high separation efficiency. This study can open a new path for the separation of colloidal particles in both research and industrial fields and further promote the development of functional nanomaterials in greener pathways.