In order to approach the single-molecule level, the molecular systems have to be organized on surfaces, where they can be approached and investigated by scanning probe techniques. Three different general concepts were used to steer the build-up of molecular nanostructures on surfaces: (i) a two-step approach with solution-based self-assembly of surpamolecules and subsequent surface deposition. (ii) one-step surface self-assembly of weak interacting organic nanostructures or (iii) surface-confined coordination chemistry of metal ions and organic ligand systems.