Preparation of strong, flexible, and multifunctional carbon-based films has attracted considerable interest not only in fundamental research areas but also for industrial applications. We report a binder-free, ultrastrong, and foldable carbon nanotube (CNT) film using aligned few-walled nanotube sheets drawn from spinnable nanotube arrays. The film exhibits tensile strengths up to 2 GPa and a Young’s modulus up to 90 GPa, which is markedly superior to other types of carbon-based films reported, including commercial graphite foils, buckypapers, and graphene-related papers. The film can bear severe bending (even being folded) and shows good structure integrity and negligible change in electric conductivity. The unique structure of the CNT film (good nanotube alignment, high packing density) provides the film with direct and efficient transport paths for electricity. As a flexible charge collector, it favors a magnesium oxide coating to exhibit high charge/discharge rate stability and an excellent electrochemical capacitance close to its theoretical value.