A simple and versatile strategy for the directed assembly of carbon nanotubes (CNTs) using side-chain functionalized poly(thiophene)s is presented. Modular variations in the side-chain of the polymers can be used to fine-tune the surface properties of polymer-wrapped CNTs, which yields CNTs soluble in either water or organic solvents. Directed assembly of the CNTs based on electrostatic interactions or metal-ligand interactions can be obtained, depending on the functional group on the side-chain of the polymers. Patterned thin films of CNTs with very high CNT density can be obtained with this approach, and the surface selectivity is extremely high. © 2013 American Chemical Society.