New methods have been developed for the synthesis and electrodeposition of functionalized single-walled carbon nanotubes (f-SWNTs). Polystyrene sulfonate functionalized nanotubes (PSS-f-SWNTs) and poly(ethylene imine) functionalized nanotubes (PEI-f-SWNTs) were co-deposited with cationic chitosan macromolecules. It was shown that chitosan promotes cathodic deposition of anionic PSS-f-SWNTs. The strategies for charging and electrodeposition of PEI-f-SWNTs include partial protonation of PEI in acidic chitosan solutions or formation of cationic Ag + –PEI complexes. The thickness of chitosan–PSS-f-SWNTs and chitosan–PEI-f-SWNTs composite films was varied in the range of up to 0.5–5μm. The amount of f-SWNTs in the deposits was varied by controlling the SWNT concentration in the solutions. It was shown that the use of chitosan enabled co-deposition of other materials, such as hydroxyapatite (HA). The proposed method enabled the fabrication of composite films.