Well-defined mesoporous TiNb6O17 microspheres are synthesized through a facile solvothermal method in isopropanol followed by a thermal treatment. The mesoporous TiNb6O17 microspheres are monodisperse with uniform morphology and are assembled by interconnected nanocrystals. The hierarchical mesoporous structure of the TiNb6O17 microspheres not only supplies a large electrode/electrolyte interfacial area but also reduces the diffusion distance of Li+, such that the TiNb6O17 microspheres have excellent electrochemical properties, especially a good rate performance. As the rate is increased from 1 to 5, 10, 20, and 30 C, the discharge capacity of the TiNb6O17 microspheres is slowly reduced from 273.7 to 239.5, 228.2, 216.0, and 175.3 mAh g−1, respectively. The good rate performance is mainly caused by the pseudocapacitive effect. These mesoporous TiNb6O17 microspheres are promising anode materials for producing lithium-ion battery with excellent rate capacity and good safety.