Self-assembly offers an attractive tool to construct well-organized π-conjugated materials. It is possible not only to study material properties at the supramolecular level, but also to tune the macroscopic properties of π-conjugated systems. Recently, several new approaches have been reported to fixate self-organized π-conjugated systems. Thermotropic and lyotropic liquid-crystalline phases of π-conjugated systems and specific conformations of polymers have been polymerized to create shape-persistent objects. Another method in this respect is to remove the solubilizing groups in an additional processing step after self-assembly. For fabricating plastic electronics devices, extra manipulation steps such as alignment layers are often required to obtain long-range order. Furthermore, vertical or homeotropic alignment of self-assembled objects is extremely difficult and is still a great challenge.