The field of organic electronics has been thriving for the last decades due to growing commercial interest. One of the advantages of using organic materials as semiconductors is the possibility to tune their optoelectronic properties by modifying the chemical structure and organization of the building blocks. In this thesis, the properties of charge carriers and excited states in a variety of organic supramolecular materials were studied in relation to the chemical structure and organization of their building blocks. The charge transport properties were studied by pulse radiolysis time-resolved microwave conductivity (PR-TRMC) measurements and theoretical calculations. The excited state properties were investigated by combining optical spectroscopy with exciton theory calculations.