Techniques for CNT solubilization and surface-selective deposition via polymer-mediated assembly are provided. In one aspect, a method for self-assembly of CNTs on a substrate is provided. The method includes the following steps. One or more surfaces of the substrate are coated with a thiol-reactive compound. The substrate is contacted with carbon nanotube-polymer assemblies dispersed in a solvent, wherein the carbon nanotube-polymer assemblies include the carbon nanotubes wrapped in a polymer having side chains with thiol groups. Wherein by way of the step of contacting the substrate with the carbon nanotube-polymer assemblies, the carbon nanotube-polymer assemblies selectively bind to the surfaces of the substrate based on an interaction between the thiol groups in the polymer and the thiol-reactive compound on the surfaces of the substrate and thereby self-assemble on the substrate.