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This thesis offers novel insights into the time-dependent structural evolution of polymers under deformation. The described results form a crucial fundament for the understanding of the sub-second deformation behavior. The thesis describes the kinetics of strain-induced crystallization in natural rubber, thus offering a new understanding of its mechanical behavior. This has become possible through the detailed scanning X-Ray diffraction investigation of the local structure around a crack tip. Karsten Brüning complements these investigations in his thesis with electron microscopy measurements. In all his experiments, he employs skillful combinations of the investigation techniques with novel sample preparation methodology. The results in this thesis expand the understanding of structure-property relationships of elastomers under deformation.