We report a new strategy to disperse single-wall carbon nanotubes (SWNTs) via conjugated moiety-containing pendant polymers, poly(2-vinylpyridine)-co-poly(9,9-dihexyl-2-(4-vinylphenyl)-9H-fluorene) (P2VP-co-P(StFl)). The polymer composition ratio and molecular weight were varied to control the SWNT dispersion. The P(St-Fl) segments were adsorbed to the surface of the de-bundled SWNTs through π–π interaction, while the P2VP segments surrounded the outer surfaces of the SWNTs to enhance their solubility and stability. A low-voltage field-effect transistor (FET) was fabricated using a P(St-Fl)-wrapped SWNT network, SWNTs wrapped with P2VP79-co-P(St-Fl)347, and hafnium oxide as the active layer, gate electrode, and dielectric, respectively. The field-effect mobility of the fabricated device was as high as 0.82 cm2 V−1 s−1 on average, with an ON/OFF ratio over 104 under a −5 V bias. This study highlights the tailored wrapping power of pendant polymers, as well as the tunable electrical conducting/semiconducting properties of SWNTs for FET device applications. The wrapping abilities of comb-like polymers with pendant conjugated fluorine moieties and their tunable electrical properties of SWNTs were discussed. It is found that longer side-chain-conjugated fluorene segments in homopolymer (P(St-Fl)300, 7) can strongly bind to the SWNTs surfaces through π–π interaction and its copolymer (P2VP79-co-P(St-Fl)347, 5a) lead to predominant dispersion of SWNTs due to the flexibility of P2VP for further increasing the solubility. Thus, SWNTs wrapped by 5a after thermal annealing can be selected as a gate electrode, whereas the spin-coated SWNTs wrapped by 7 can be as a semiconductor for the FET channel, resulting in a mobility of 0.82 cm2 V−1s−1, a threshold voltage of 0.35 V and an ON/OFF ratio of 2.8 × 104.