Although the large 'melt elongation' of polymers should significantly affect crystallization that controls the structure and properties of solids, it has been difficult due to technical reasons. In this paper, we succeeded in bulky elongational crystallization of isotactic polypropylene (iPP) by compressing the supercooled melt. The crystallization behavior and structure were observed by means of optical microscope, transmission electron microscopy (TEM) and X-ray scattering. When the elongational strain rate ( . e) surpassed a critical value ( . e*¼2Â10 2 s À1 ), the crystallization behavior, structure and physical properties underwent a discontinuous change. The crystallization rate increased by a factor as large as 10 6 , the crystallite lateral size decreased by a factor of 10 À3 to 20-30 nm and the morphology changed from well-known spherulites to a novel morphology of 'nano-oriented crystals (NOCs)'. These NOCs showed a high crystallinity (nearly equal to unity). The above results indicate that the polymer melt changed from isotropic to 'oriented melt' which accelerated nucleation and growth rates and induced NOC formation. NOCs showed ultra-high performance such as high tensile strength at break (D2.1Â10 2 MPa), comparable to that of metals, and a high thermal resistance (D176 1C). NOCs will be useful in a wide variety of applications and will contribute to efforts to construct a sustainable society by enabling the development of lightweight, recyclable materials. Polymer Journal (2010) 42, 464-473; doi:10.1038/pj.2010.35Keywords: crystallization; elongation; isotactic polypropylene; nano; SAXS; WAXS INTRODUCTION String-or chain-like molecules are major constituents of natural materials, as they have the remarkable characteristic of a high ability to self-organize. Because these molecules can form complex structures, they perform multiple functions and can carry information. The functions of these molecules and the information they carry have evolved over more than three billion years. Chain-like materials, called polymers, are now used in a variety of applications and have properties similar to those of the natural string-like molecules discussed above. Therefore, it is important for us to understand and control the behaviors of the structure formation of polymer.The molecular chain of a polymer in a melt or solution significantly changes its shape if an external field, such as an elongation, changes from weak to strong one, 1 which should significantly affect the crystallization behavior and properties of polymer solids. Therefore, the mechanism of structure formation and the expression of function of polymers under strong elongational fields are interesting problems