Supramolecular self-assembly of organic materials is an interesting alternative for the bottom-up design of organic devices. By using desired supramolecular interactions such as hydrogen bonding, π-π stacking, electrostatic interactions, and other nonconvalent interactions, scientists have begun taking control of the nanoscale ordering of the active layer. Synthetic and supramolecular strategies enable us to construct functional molecular architectures for devices. This review describes current progress in organic light-emitting (OLED) and photovoltaic (OPV) devices in which the molecular components possess designed supramolecular interactions – as opposed to non-specific cohesive forces – used to instill or modify functionality.