We describe herein a high-yield method to selectively disperse semiconducting CoMoCAT (CO disproportionation on Co-Mo Catalysts) single-walled carbon nanotubes (SWNTs) with regioregular poly (3-alkylthiophenes) polymers. We observed that the dispersion yield was directly related to the length of the polymer's alkyl side chains. Molecular dynamics simulations in explicit toluene (real toluene molecules) indicate that polythiophenes with longer alkyl sidechains bind stronger to SWNTs, due to the increased overall surface contact area with the nanotube. Furthermore, the sorting process selectively enriches smaller-diameter CoMoCAT SWNTs with larger bandgaps, which is ideal for solar cell applications. Compared to the larger diameter sorted HiPco (High-Pressure CO) SWNTs, solar cells fabricated using our sorted CoMoCAT SWNTs demonstrated higher open-circuit voltage (Voc) and infrared external quantum efficiency (EQE). The Voc achieved is the highest reported for solar cells based on SWNT absorbers under simulated AM1.5 solar illumination. Additionally, we employed the sorted CoMoCAT SWNTs to fabricate thin film transistors with excellent uniformity and device performance.