Motivated by the persistent desire for (novel) materials, which exhibit currently unavailable functionalities, research focused on the creation of polymers with tailored properties has evolved to a central field at the interface of chemistry, materials science, and physics. Polymers, as a group of materials, often offer an attractive combination between ease of processing and final properties. Especially the ability to design their chemical structure virtually at will but also the possibility to control the often very rich phase behavior and supramolecular architectures of polymer systems allows one to minutely tailor the properties of this remarkable class of materials. At hand of selected examples, which include semi-conducting conjugated polymer networks, molecular strain sensors, and artificial sea cucumbers, our current activities regarding the development and investigation of new photo- and electrofunctional polymers are summarized.