Lithium-ion batteries (LIBs) with a Li4Ti5O12 (LTO) anode offer an attractive solution for large-scale energy storage applications because of the high safety, excellent cycle life, and rate capability. However, the low storage capacity of LTO (~160 mAh g-1) has limited its further application. Here, we report a facile approach to prepare nanoporous TiNb2O7 anode materials with a similar average storage voltage, but much higher storage capacity (281 mAh g-1) than well-known Li4Ti5O12 (~160 mAh g-1). The interconnected nanoporous framework composed of nanocrystals leads to drastically enhanced rate (a capacity retention of 70% at 20 C) and cycling performance (a very small capacity decay of 0.016% per cycle over 1000 cycles) with very high coulombic efficiency (around 100%). The present report demonstrates significant progress toward the development of TiNb2O7 based long-life stationary lithium-ion batteries with high energy density.