Strain-induced crystallization (SIC) of natural rubber (NR) samples with different strain rates at a fixed strain was investigated by synchrotron radiation X-ray diffraction measurements, which provided the evolution trends of crystal sizes and crystallinity during the SIC process. It was found that the Avrami index was about 1 during the crystallization of NR after the cessation of stretch, which demonstrated that sporadic nucleation occurred during SIC process. The increase of the crystallinity was attributed to the increase of the number of new crystallites rather than the growth of the crystal size. An unexpected relationship between the final crystallinity and the strain rates was observed. The increase of physical crosslink points originated from either entanglement or crystallite was considered as the reason that leads to the nonmonotonic variation of the final crystallinity with strain rates. (c) 2012 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2012