AbstractTiO2 nanohybrid material with pillared nanostructure is prepared via an exfoliation/reassembly process of exfoliated Ti0.91O2 nanosheets and TiO2 nanoparticles, followed by a calcination treatment. The as‐prepared material consists of TiO2 nanoparticles (≈5–8 nm) randomly distributed in the interlayers of reassembled TiO2 nanosheets, resulting in a high specific surface area of 207 m2 g−1, which can effectively facilitate lithium diffusion and accommodation. The formed disordered TiO2 pillared material can deliver a specific discharge capacity of 349 mA h g−1 at 0.2 C with sufficient lithium intercalation and exceptional cycling stability for up to 150 cycles, and survive more than 350 continuous cycles with almost no capacity fading at 1 C, 5 C and 10 C. The superior electrochemical properties of our TiO2 nanohybrids demonstrate sufficient and reversible lithium insertion/extraction, and ultrafast lithium diffusion and storage capabilities.