DNA molecules are well known for containing the genetic information of an individual. Furthermore, DNA is a biopolymer with the potential of building up nanoscale structures. These structures can be addressed sequence specifically and, therefore, they allow connecting and arranging with subnanometer accuracy. The extended work of the group of Nadrian Seeman (Nature 421:427–431, 2003) has shown that the self-assembly of DNA molecules offers great potential for the creation of bottom-up nanostructures for nanoelectronics, biosensors, and programmable molecular machines. Rothemund (Nature 440:297–302, 2006) has shown that it is possible to generate a wide variety of 2D nanostructures by the assembly of synthetic desoxyoligonucleotides and M13mp18 DNA via Watson–Crick base pairing . Furthermore, DNA can form three- and four-stranded structures which offer even more possibilities for molecular construction. This chapter will deal with four-stranded DNA structures (G-wires) created from 10-bp deoxynucleotide units. Our focus will be especially on the synthesis, individualization, modification with gold nanoparticles, and characterization by high-resolution scanning force microscopy (AFM).