Amine-terminated self-assembled monolayers (SAMs) can be utilized to selectively adsorb semiconducting single-walled carbon nanotubes (S-SWNTs), but are not ideal. Formation of these monolayer films from silanes can be dramatically influenced by atmospheric and other processing conditions, resulting in poor-quality SAMs or irreproducible results. The surface sorting method of fabricating these semiconducting nanotube networks (SWNTnts) can become ineffective if the functionalized surface is not smooth with high amine density. However, by replacing the amine with a nitrile group, SAM formation can be made more controllable and reproducible. Upon SWNT deposition, the nitrile group was found to not only adsorb higher density SWNTnts but also sort the nanotubes efficiently, as shown by micro-Raman spectroscopy. Upon testing these SWNTnts for device performance, these thin-film transistors (TFTs) were also found to yield higher quality devices than those fabricated on amine surfaces. Overall, these results expand the applicability of surface sorting and SWNT adsorption to other organic functionalities for nanotube separation. This report provides an outline of the merits and characterization of using the nitrile functional group for the separation and adsorption of SWNTs and its integration in network TFTs.