Spinel-type Li4Ti5O12 has been proposed as an advanced anode for energy storage because of its safety and stability in recent years. However, the Li4Ti5O12 anode reported so far exhibited poor rate performance and required further improvement. Herein, a highly conductive network with PPy polymer and N-doped graphene sheet is constructed with Li4Ti5O12 embedded inside for the first time. In this design, the Li4Ti5O12 particles are uniformly coated with conducting PPy layer and further connected by the N-doped graphene. This combined structure is favorable to facilitate the electron and Li+ transmission, and thus enhance the battery performance. The as-fabricated composite delivers the initial capacities of 186.2 and 152.9 mAh g−1 at 0.1 and 10 C, respectively. The above results reveal that the conducting PPy polymer and N-doped graphene sheet co-modified Li4Ti5O12 composite would be a potential anode for next-generation energy storage device.