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This thesis offers novel insights into the time-dependent structural evolution of polymers under deformation. In-situ tensile experiments at high-brilliance synchrotron sources allowed to characterize the material with unrivaled resolution in time and space. The strain-induced crystallization in natural rubber was studied by wide-angle X-ray diffraction. Special emphasis was put on the establishment of new structure-property relationships to give a more in-depth understanding of the mechanical performance of rubber parts, e.g. in tear fatigue loading. To this end, the kinetics of...