Fullerene molecules are interesting materials because of their unique structures and properties in mechanical, electrical, magnetic, and optical aspects. Current research is focusing on the construction of well-defined fullerene nano/microcrystals that possess desirable structures and morphologies. Further tuning the intermolecular interaction of the fullerene nano/microcrystals by use of pressure is an efficient way to modify their structures and properties, such as creation of nanoscale polymer structures and new hybrid materials, which expands the potential of such nanoscale materials for direct device components. In this paper, we review our recent progress in the construction of fullerene nanostructures and their structural transformation induced by high pressure. Fullerene nano/microcrystals with controllable size, morphology and structure have been synthesized through the self-assembly of fullerene molecules by a solvent-assisted method. By virtue of high pressure, the structures, components, and intermolecular interactions of the assemblied fullerene nano/microcrystals can be finely tuned, thereby modifying the optical and electronic properties of the nanostructures. Several examples on high pressure induced novel structural phase transition in typical fullerene nanocrystals with C60 or C70 cage serving as building blocks are presented, including high pressure induced amorphization of the nanocrystals and their bulk moduli, high pressure and high temperature (HPHT) induced polymerization in C60 nanocrystals, pressure tuned reversible polymerization in ferrocene-doped C60/C70 single crystal, as well as unique long-range ordered crystal with amorphous nanoclusters serving as building blocks in solvated C60 crystals, which brings new physical insight into the understanding of order and disorder concept and new approaches to the design of superhard carbon materials. The nanosize and morphology effects on the transformations of fullerene nanocrystals have also been discussed. These results provide the foundation for the fabrication of pre-designed and controllable geometries, which is critical in fullerenes and relevant materials for designing nanometer-scale electronic, optical, and other devices. Fullerene molecules are interesting materials because of their unique structures and properties in mechanical, electrical, magnetic, and optical aspects. Current research is focusing on the construction of well-defined fullerene nano / microcrystals that possess desirable structures and morphologies. Further tuning the intermolecular interaction of the fullerene nano / microcrystals by use of pressure is an efficient way to modify their structures and properties, such as creation of nanoscale polymer structures and new hybrid materials, which expands the potential of such nanoscale materials for direct device components. In this paper, we review our recent progress in the construction of fullerene nanostructures and their structural transformation induced by high pressure. Fullerene nano / microcrystals with controllable size, morphology and structure have been synthesized through the self-assembly of fullerene molecules by a solvent-assisted method. virtue of high pressure, the structure s, components, and intermolecular interactions of the assemblied fullerene nano / microcrystals can be finely tuned, thereby modifying the optical and electronic properties of the nanostructures. Several examples on high pressure induced novel structural phase transition in typical fullerene nanocrystals with C60 or C70 cage serving as building blocks are presented, including high pressure induced amorphization of the nanocrystals and their bulk moduli, high pressure and high temperature (HPHT) induced polymerization in C60 nanocrystals, pressure tuned reversible polymerization in ferrocene-doped C60 / C70 single crystal, as well as unique long-range ordered crystal with amorphous nanoclusters serving as building blocks in solvated C60 crystals, which brings new physical insight into the understanding of order and disorder concept and new approaches to the design of superhard carbon materials. The nanosize and morphology effects on the transformations of fullerene nanocrystals have also been discussed. These results provide the foundation for the fabrication of pre-designed and controllable geometries, which is critical in fullerenes and relevant materials for designing nanometer-scale electronic, optical, and other devices.