The structure and properties of single macromolecules are key to understanding function in biologicalmolecular systems, as well as to developing artificial functional systems. In order to systematicallyinvestigate and control the conformations of single macromolecules and their complexes a “molecularworkbench” has been developed. It consists of an atomically flat, inert solid substrate suchas the basal plane of highly oriented pyrolytic graphite (HOPG), coated with a layer of moleculessuch as alkanes or alkyl chains containing amphiphiles that control the interaction between the substrateand adsorbed macromolecules. A scanning force microscope (SFM) operated in tapping or contactmode is used to both image and manipulate the macromolecules to correlate their structure with mechanicalproperties, and to assemble macromolecular systems that would not form spontaneously.