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DNA performsa vital function as a carrier of genetic code, but in the field ofnanotechnology, DNA molecules can catalyze chemical reactions in thecell, that is, DNAzymes, or bind with target-specific ligands, thatis, aptamers. These functional DNAs with different modifications havebeen developed for sensing, imaging, and therapeutic systems. Thus,functional DNAs hold great promise for future applications in nanotechnologyand bioanalysis. However, these functional DNAs face challenges, especiallyin the field of biomedicine. For example, functional DNAs typicallyrequire the use of cationic transfection reagents to realize cellularuptake. Such reagents enter the cells, increasing the difficulty ofperforming bioassays in vivo and potentially damaging the cell’snucleus. To address this obstacle, nanomaterials, such as metallic,carbon, silica, or magnetic materials, have been utilized as DNA carriersor assistants. In this Account, we describe selected examples of functionalDNA-containing nanomaterials and their applications from our recentresearch and those of others. As models, we have chosen to highlightDNA/nanomaterial complexes consisting of gold nanoparticles, graphene oxides, and aptamer–micelles, and we illustrate the potentialof such complexes in biosensing, imaging, and medical diagnostics. [ABSTRACT FROM AUTHOR]