High-tap density electrode materials are greatly desired for Li-ion batteries with high volumetric capacities to fulfill the growing demands of electric vehicles and portable smart devices. TiO2, which is one of the most attractive anode materials, is limited in their application for Li-ion batteries because of its low tap density (usually <1 g cm −3 ) and volumetric capacity. Herein, we report uniform mesoporous TiO2 submicrospheres with a tap density as high as 1.62 g cm −3 as a promising anode material. Even with a high mass loading of 24 mg cm −2 , the TiO2 submicrospheres have impressive volumetric capacities that are more than double those of their counterparts. Moreover, they can be synthesized with 100% yield and within a reaction time of~6 h by optimizing the experimental conditions and formation mechanism, exhibiting potential for large-scale production for industrial applications. Other mesoporous anode materials, i.e., hightap density mesoporous Li4Ti5O12 submicrospheres, are fabricated using the generalized method. We believe that our work provides a significant reference for the industrial production of mesoporous materials for Li-ion batteries with a high volumetric performance.