The present work explored the structure-property correlations for the biopolymer poly(L-lactic acid) (PLA) by studying deformation-mediated molecular orientation and crystallization. The structural and morphological variations of amorphous PLA under different strain rates were investigated. The result showed that strain rate significantly influences its strain-hardening behavior. The crystallinity and orientation as well as cavitation of deformed PLA increase with the increase of strain rates. The structure evolution has been divided into three potential stages: (i) at small strains (<100%), the crystallinity of PLA increases by orientation-induced crystallization; (ii) at intermediate strains (100%-160%), the crystallinity of deformed PLA slightly decreases due to the breakage of existing crystals under stress accompanying with newly formed voids and cavities; (iii) at high strains (>160%), the increasing number of oriented chains in the amorphous regions promotes the crystallization of PLA. Our study suggests that strain rate and stretching strain play important roles on modulating the crystallization and orientation of amorphous PLA. (C) 2011 Elsevier Ltd. All rights reserved.