The growth of ultrathick shells on quantum dots (QDs) has been demonstrated to provide new aspects of nanoparticles (NPs). Spherical dot-shaped CuInSe2 QDs were produced with the advantage of shell growth due to their homogeneous surface. The superthickness (∼45 nm) of CuInS2 was deposited on the CuInSe2 dots to form supersized CuInSe2/CuInS2 core/shell nanostructures with a tetrakaidecahedron shape to ∼100 nm. This quasi-epitaxial growth mechanism was extended to form supersized ZnSe/CuInS2 and CuInS2/CuInS2 core/shell nanostructures, thereby providing an efficient method for supersized nanoparticles based on shell growth. The formation of supersized nanoparticles (20-100 nm) may induce new chemistry and physics for nanomaterials, supplying new aspects in fundamental research and the commercial industry.