The present theoretical exploration provides initial guidance for experimental realization of programmability, via ssDNA "functionalization", for achieving self-assembled carbon-based architectures for nanoelectronics. Indeed, early attempts indicate that DNA functionalization of nanocarbons, such as graphene or CNTs 25 may be possible although a synthetically challenging task. Quantum transport calculations also suggest that such components, even in presence of hydrogen-bonded junctions, may adequately function as electron transport media between GNRs. DNA-functionalization may also improve upon existing liquid-phase processing methods in creating highly compact and aligned nanosheets for electronics. This molecular precision of nanosheet assembly can be accomplished both in 2D and potentially 3D via the incorporation of multiple different DNA sequences on one edge 56 and the use of flexible linkers that enable additional shape (instead of solely chemical) complementarity. Our results also have an interesting parallel to naturally assembled structures. Years of evolution have determined that three nucleotides are optimal and sufficient to specify codons that can generate an overwhelming diversity of proteins and biological structures. Similarly, we suggest that the energy scales associated with DNA specify an optimal size and heterogeneity of sequences that can reliably self-assemble into a diverse gamut of complex nanostructures.