Poly(3-hexylthiophene) (P3HT) has received much attention as a good candidate to replace inorganic semiconductors for flexible electronics due to its solution-processability. However, the low charge mobility of P3HT is an obstacle to its commercialization. To overcome this problem, we propose a new non-covalent functionalization method for carbon nanotubes (CNTs) for use in CNT/P3HT nanocomposites. By using modified pyrene molecules with hydrophobic long alkyl chains, the non-covalently functionalized CNTs can become well dispersed in hydrophobic solutions and organic semiconductor matrices. Fabrication of organic thin-film transistors (OTFTs) from the non-covalently functionalized CNT/organic semiconductor nanocomposites shows that our non-covalent functionalization method significantly reduces damage to CNTs during functionalization when compared with covalent functionalization by treatment with acids. The OTFTs show 15 times enhancement of field effect mobility (1.5 × 10⁻² cm²/(V·s)) compared to the mobility of OTFTs made from pure P3HT. This enhancement is achieved by addition of only 0.25 wt% of CNTs to P3HT.