C60 crystals have potential applications in the optoelectronics, photoconducting devices and templated synthesis fields. However, their preparation is complex. A simple liquid-liquid interfacial precipitation method was used to fabricate hierarchically-organized C60 crystals with various topographic characteristics, using 1,2,3,4-tetrahydronaphthalene as a good solvent, and isopropanol, ethanol or methanol as a poor solvent. Results indicate that the morphology and shape of the as-prepared C60 crystals vary according to the solvent combination and the ratio of good to poor solvents. The SEM images of fractured surfaces and XRD patterns of the crystals reveal that the crystals are formed by the hierarchical organization of C60 molecules at the molecular level to nanocrystals that are assembled into micrometer crystals. The crystals are composed solely of C60 molecules, without polymerization and solvents, which are arranged in a face-centered cubic lattice. The surface roughness is increased by post washing with ethanol. The methodology described here is advantageous over the high-temperature conversion and solvent annealing methods reported previously.