Compared to single-walled carbon nanotubes (SWNTs) and more defective multiwalled carbon nanotubes (MWNTs), the thin few-walled carbon nanotubes (FWNTs) are believed to have extraordinary mechanical properties. However, the enhancement of mechanical properties in FWNTs-polymer composites has remained elusive. In this study, free-standing carbon nanotubes (CNTs)/polymer composite films were fabricated with three types (SWNTs, FWNTs, MWNTs) of functionalized CNTs. The mechanical properties of composite films have been investigated. It is observed that the Young’s modulus of composite films with only 0.2 wt % functionalized FWNTs shows a remarkable reinforcement value of dY/dVf = 1658 GPa, which is 400 GPa higher than the highest value (dY/dVf = 1244 GPa) that was previously reported. In addition, the Young’s modulus increased steadily with the increased concentration of FWNTs. The results indicated that FWNTs are practically the optimum reinforcing filler for the next generation of carbon nanotube-based composite materials.