Nanotubes to Order To exploit carbon nanotubes fully in electronic applications, one needs to be able to separate or synthesize either all semiconducting or all metallic tubes. However, unbiased synthesis conditions produce a mixture containing two-thirds semiconducting tubes and one-third metallic tubes. Harutyunyan et al. (p. 116) show that altering the carrier gas and temperature, in combination with oxidative and reductive species during the synthesis process modifies the catalyst particles during synthesis, which leads to the selective growth of metallic single-walled carbon nanotubes. Thus, the shape and morphology of the catalyst seeds can be tuned to grow carbon nanotubes of a specific chirality. Reaction conditions that alter catalyst particles can bias the chirality and electronic properties of nanotube products. Single-walled carbon nanotubes can be classified as either metallic or semiconducting, depending on their conductivity, which is determined by their chirality. Existing synthesis methods cannot controllably grow nanotubes with a specific type of conductivity. By varying the noble gas ambient during thermal annealing of the catalyst, and in combination with oxidative and reductive species, we altered the fraction of tubes with metallic conductivity from one-third of the population to a maximum of 91%. In situ transmission electron microscopy studies reveal that this variation leads to differences in both morphology and coarsening behavior of the nanoparticles that we used to nucleate nanotubes. These catalyst rearrangements demonstrate that there are correlations between catalyst morphology and resulting nanotube electronic structure and indicate that chiral-selective growth may be possible.