Ti2Nb10O29 (TNO) is a prospective anode for lithium-ion batteries (LIBs) because of its high theoretical capacity, high energy density, and safer operating voltage. However, the lower conductivity and slower lithium-ion diffusion characteristic lead to performance degradation and accelerated capacity degradation. In this work, we developed a novel and simple urea-assisted heat treatment method to enrich oxygen vacancies in TNO anodes. Oxygen vacancy introduction leads to the formation of Ti3+ and Nb4+ and the optimization of electronic structure, which provide more active sites for ion insertion and accelerate electron transport and migration. The optimized sample (TNO-M) demonstrates excellent high-rate capacity and cyclic stability. Specifically, the reversible capacity is 155.4 mAh/g at 10C. A capacity retention ratio of 97.87 % can be maintained after 200 cycles at 1C. Even after 500 cycles at 5C, TNO-M can still deliver a high capacity of 156.4 mAh/g. The strategy of developing high-capacity and high-rate anodes provides a new inspiration for the applications of fast charging of energy-dense LIBs.