Terpyridines represent versatile functional supramolecular building blocks that are easily integrated in numerous devices and can readily modify surfaces. In particular, redox-active complexes with terpyridine ligands have been attached to surfaces, either by covalent or non-covalent interactions, and form highly ordered mono- or multilayer systems, since electronic and charge transport properties are major topics of interest. Their applications in nanoelectronics are a driving force for understanding and enabling the utilization of the supramolecular properties of terpyridines for surface modification. This area of research has received increasing attention during the last decade leading into the supramacromolecular regime. This Progress Report presents an overview of the state-of-the-art of surface modifications utilizing terpyridine systems and highlights main results, as well as modern trends, in this research area.