The invention discloses a method for phase transferring and three-dimensional assembling of precious metal nano-particles. The method comprises the following steps that after centrifugation is carried out on the aqueous solutions of the precious metal nano-particles, the aqueous solutions of 2 (diethyl aminoethyl acyl methyl ethyl) octadecylamine are added to sediments acquired through the centrifugation for ultrasonication, obtained dispersion liquid and the organic solutions of the 2 (diethyl aminoethyl acyl methyl ethyl) octadecylamine are mixed and vibrated, standing is carried out, and the precious metal nano-particles are transferred from a water phase to an oil phase. Centrifugation is carried out on the precious metal nano-particles transferred to the oil phase for the first time, the organic solutions of the 2 (diethyl aminoethyl acyl methyl ethyl) octadecylamine are added to the sediments acquired through the centrifugation for the ultrasonication, then obtained dispersion liquid and the organic solutions of silicon dioxide balls decorated by sulfydryl are mixed and stirred, centrifugation is carried out for the second time, obtained sediments are the precious metal nano-particles after the three-dimensional assembling, and the three-dimensional assembling of the precious metal nano-particles is achieved. The method is simple in operation, balance time for the phase transferring is short, and repeatability and controllability are better.