The pioneering work of Heeger MacDiarmid, and Shirakawa, rewarded by the 2000 Nobel Prize in Chemistry, has paved the way for the development of the fields of plastic electronics and photonics. Functional organic molecular materials and conjugated oligomers or polymers now allow the low-cost fabrication of thin films for insertion into new generations of electronic and optoelectronic devices. The performance of these devices relies on the understanding and optimization of several complementary processes (see sketch). Our goal is to discuss, from a theoretical standpoint, the electronic structure characteristics and interfacial properties that are of importance in all these areas. The concept of interface should be taken here in the microscopic sense, i.e., molecular interactions among two or several chains/molecules (of the same or of a different nature). Specifically, we will address the impact of interchain interactions within an organic layer on the transport and optical properties. These issues will therefore be more directly related to transistor and light-emitting diode applications; however, in all instances, the aspects related to interfacial charge or energy transfer processes will dictate the ultimate performance of a material in a given device.