ABSTRACT:Strain-induced crystallization (SIC) of natural rubber (NR) has been extensively studied even before the advent of macromolecular physics. However, there are still some unsolved basic issues in this field. In this review article, classic studies on SIC of NR are briefly introduced, and then recent results by synchrotron X-ray diffraction studies in separate papers by different authors are categorized and interpreted on the basis of molecular models. Cyclic deformation experiments provided information on partial orientation of the network-chains, on nucleation and morphological changes of crystals and on stress field around the strain-induced crystals. On the other hand, experiments under constant strain provided information on kinetics of SIC, on stress relaxation due to SIC, and so on. The experimental results could be explained under the assumption that the SIC is dominated by strain, and that the crystals are of foldedchain type. However, in order to consistently explain the various experimental results, we have to establish a unified molecular model of the network structure. [doi:10.1295/polymj.PJ2007059] KEY WORDS Network-chain Density / Crosslinking / Supercooling / Entropy / Rubber Elasticity / Crystallite Size / Entanglement / Natural rubber (NR) from Hevea latex is an indispensable material for many industrial and household applications, 1 which is constituted of cis-1,4-polyisoprene (ca. 94%) and non-rubber components such as proteins (ca. 2%) and lipid (ca. 3%).2 The versatility of the plant-derived NR is mainly due to its outstanding tensile properties and the good crack growth resistance. We still cannot reproduce the good performance of the NR products using synthetic cis-1,4-polyisoprene rubber (IR). The superiority of NR has been thought to originate from its ability to crystallize immediately by expansion; by contrast, crystallinity of IR is not as high as NR because of the lower regularity of the main-chain structure. 2,3 In this context, straininduced crystallization (SIC) of NR has been extensively studied even before the advent of macromolecular physics.