One of the ultimate miniaturizations in nanotechnology is molecular electronics, where devices will consist of individual molecules. There are many complications associated with the use of molecules in electronic devices, such as the electronic perturbations in the molecule associated with being bonded to an electrode, how electrons traverse the metal-molecule junction, and the difficulty of macroscopically addressing single to very few molecules. Whether fabricating a test structure or a usable device, the use of self-assembly is fundamental to the fabrication of molecular electronic devices. We will discuss how to fabricate self-assembled monolayers into test assemblies and how to use intermolecular interactions to direct molecules into desired positions to create nanostructures and to connect functional molecules to the outside world. These assemblies serve as test structures for measurements on single or bundled molecules. The development of several experimental techniques, including various scanning probes, mercury drop junctions, break junctions, nanopores, crossed wires, and other techniques using nanoparticles have enabled the ability to test these structures and make reproducible measurements on single molecules. Many of these methods have been developed to test molecules with potential for integration into devices such as oligo (phenylene-ethynylene) molecules and other π-conjugated molecules, in ensemble or single-molecule measurements.