Flexible and durable electrode materials are of vital importance to developing advanced energy storage devices for emerging wearable electronics. Most current strategies adopt chemical modifications or chemical binders to improve the interface interaction between flexible components, which inevitably lowers the cyclic lifetime and increases the production cost. Here, we report an in situ, scalable sol–gel method to fabricate free-standing TiO2/superaligned carbon nanotube (SACNT) hybrid films as flexible anodes in Li-ion batteries. The natural and desirable wettability between TiO2 and SACNTs makes any chemical modifications or chemical binders unnecessary in the fabrication process, delivering a clean TiO2–SACNT interface. The as-prepared TiO2/SACNT anodes not only inherit the high flexibility of the SACNT framework but also enhance rate capability and charge/discharge reversibility with its pseudocapacitive storage mechanism. These anodes exhibit a high capability and a long cyclic lifetime (over 1000 c...