Carbon nanotubes have long been of interest as additives for increasing the mechanical and electronic properties of polymers, and considerable progress has been made.[1±6] However, melt-phase and solution viscosities ordinarily become too high for conventional processing when the nanotube component exceeds about 10 wt.-%, which limits the nanotube contribution to composite properties. In a groundbreaking development, Vigolo et al. have shown that composite fibers comprising largely nanotubes can be obtained by a process called polyvinyl alcohol (PVA) coagulation spinning. [7±9] In this process, a dilute surfactant-assisted single-walled carbon nanotube (SWNT) dispersion is coagulated into a gel state by spinning it into an aqueous PVA solution; this is followed by conversion into a solid fiber by a slow draw process, during which the water in the gel evaporates. [7±9] We recently reported improvements in this fiber-spinning technique that dramatically increased fiber strength and fiber-spinning rate.[10±12]These improved fibers (comprised of about 60 % SWNTs in a PVA matrix) have a capacity to absorb energy (a specific toughness of about 600 J g ±1 ) that is much higher than any other natural or synthetic organic fiber. Additionally, these SWNT fibers have been successfully utilized in the fabrication of electrochemical devices, such as electromechanical actuators [1,12] and supercapacitors. [10,11] However, unless the polymer is removed by pyrolysis (which degrades the mechanical properties of the fiber), performance of these electrochemical devices is limited by the low electrical conductivity of the nanotube/polymer composite fibers and degradation of mechanical stability when the PVA in these fibers is converted into an ionic conductor. [11] We show here that fibers with useful mechanical properties can be spun if we replace the PVA coagulant with a polyethyleneimine (PEI) coagulant. Although the PEI used is ordinarily a liquid at room temperature, it interacts with the nanotubes to serve as an intertube binding agent. The resulting strain-to-failure and toughness of the PEI-containing fibers are far greater than those of the thermally annealed, binder-free SWNT fibers (which have the advantage of a somewhat higher tensile strength and electrical conductivity) that were spun using the pioneering superacid method developed by the Rice group. [13,14] While the fiber strength and toughness achieved here are far less than those of fibers obtained from the continuous spinning process of Dalton et al. for producing SWNT/PVA composite fibers, [10,11] the prospects of improving the mechanical properties of the SWNT/PEI fibers appear good. Moreover, the electrical conductivity of the SWNT/PEI composite fibers is over a hundred times that of the supertough SWNT/PVA composite fibers. PEI and, in general, amines, are known to effectively interact with carbon nanotubes via physisorption on the nanotubes' sidewalls.[15±21] Thus, a method for separating metallic and semiconducting SWNTs has been developed that uses the hi...