Motivated by the technological possibilities of electronics and sensors based on gold nanoparticles (Au NPs), we investigate the selective assembly of such NPs on electrodes via DNA hybridization. Protocols are demonstrated for maximizing selectivity and coverage using 15mers as the active binding agents. Detailed studies of the dependences on time, ionic strength, and temperature are used to understand the underlying mechanisms and their limits. Under optimized conditions, coverage of Art NPs on Art electrodes patterned on silicon dioxide (SiO2) substrates was found to be similar to 25-35%. In all cases, Au NPs functionalized with non-complementaryDNA show no attachment and essentially no nonspecific adsorption is observed by any Au NPs on the SiO2 surfaces of the patterned substrates. DNA-guided assembly of multilayers of NPs was also demonstrated and, as expected, found to further increase the coverage, with three deposition cycles resulting in a surface coverage of approximately 60%.