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TiNb2O7 (TNO) is a promising anode material for lithium‐ion batteries because of its high capacity and long cyclic life. Nevertheless, its practical application is limited by sluggish ionic and electronic conductivity. Alien ion doping is one of the most simple and effective methods to optimize the electrochemical performance of anode materials. Herein, H2MoO4 derived Mo‐doped TiNb2O7 (Mo‐TNO) microspheres have been synthesized via a solvothermal method followed by calcining process. The resulting Mo‐TNO displays an excellent rate capacity (about 200 mAh g−1 at 10 C) and a high capacity retention (80 % after 500 cycles at ∼2.6 C compared with the second cycle). In addition, the H2MoO4‐derived Mo‐TNO still keeps the microsphere shape after 500 cycles at 10 C. These superior properties demonstrate that Mo‐TNO has great application advantages as anode material for lithium‐ion batteries. [ABSTRACT FROM AUTHOR]