The versatility and rich functionality of living cells in Nature inspire researchers from many disciplines. For example, artificial replication of photosynthesis, which is an efficient solar-to-chemical energy conversion process in plants, promises a breakthrough in reducing our dependence on exhaustible and environmentally harmful fossil energy sources. I will discuss several novel concepts in bioinspired molecular electronics and optoelectronics recently enabled by the controlled self-assembly of artificial organic molecules into functional architectures with preprogrammed photo-physical properties. The molecular-scale picture of the underlying fundamental physical processes such as the photo-excited states relaxation, energy and charge carrier transport, and interfacial charge transfer, in these self-assembled heterogeneous architectures will be described. Finally, I will address current challenges and future prospects of this rapidly-expanding interdisciplinary field.