Beyond conventional organic thin-film transistors, this thesis explores possible paths for the fourth wave of organic electronics. In this context, mixed ionic-electronic conductors and organic electro-chemical transistors (OECTs) are identified as highly promising approaches for electronic bio-interfaces enabling ultra-sensitive detection of biological signals. Furthermore, these systems show fundamental properties of biological synapses, namely the synaptic plasticity, which renders the possibility to build brain-inspired, neuromorphic networks enabling highly efficient computing. In particular, the combination of OECTs acting as sensor units and self-learning neural networks at once enables the development of intelligent tags for medical applications. Overall, this thesis adds substantially new insight into the field of organic electronics and draws a vision towards further research and applications. The advancements in the field of vertical organic transistors open new perspectives for the implementation of organic transistors in high-resolution AMOLED displays or radio-frequency identification tags. Furthermore, the exploration of OECTs for neuromorphic computing will create a whole new research field across the disciplines of physics, material, and computer science.