A novel liquid–liquid interfacial precipitation (LLIP) method to prepare C 60 fullerene nanotubes (FNTs) effectively and controllably was demonstrated. It offered a simple way by mixing the ultrasounded C 60 solution and mother liquid without ultrasound treatment, which offers nuclei and supplies primitives to fabricate FNTs, respectively. The results showed that producibility of FNTs was dramatically increased by introducing ultrasound treatment to LLIP method. When the C 60 solution with ultrasound treatment and the mother liquid without ultrasound treatment are mixed together with a volume ratio of 1:9 in N-methyl-2-pyrrolidone (NMP) system, 100% of tube-content can be achieved. Meanwhile, a possible formation mechanism of FNTs was proposed, reasonably based on the experimental data.