The aim of the presented work was to elaborate the relationship between the macromolecular architecture, the morphology and the macroscopic properties of polymers that exhibit more than one phase and, thus, to contribute to the elucidation of structure-property relationships of different polymer systems. Moreover, the obtained knowledge should be used to tailor these polymers with respect to their typical applications. The investigated polymers range from commodity plastics, like olefin ethylene-co-octene copolymers (EOCs), technical polymers, like the styrene-butadiene block copolymers, up to functional polymers, like the piezoelectric P(VDF-co-TrFE) or the semi-crystalline block copolymer PB-b-PEO. The obtained results underline the impact of the morphology in polymeric multi-phase system on the achievable mechanical and electro-mechanical properties. Within this work, various analysis techniques were employed. Only by a combination of the applied techniques, essential information about the structure-property relationship can be achieved.