Achieving lithium‐ion batteries (LIBs) with ultrahigh rate at ambient‐temperature and excellent low temperature‐tolerant performances is still a tremendous challenge. In this paper, we design a binder‐free Li4Ti5O12 (LTO) electrode to achieve an excellent rate performance (∼75 % of its theoretical capacity at 200 C), in which, aligned CNT nanosheets were used to load LTO nanosheets decorated with silver nanocrystals. With combination of 1,3‐Dioxlane‐based electrolyte, there is nearly no initial voltage drop happen, and the capacity can be greater than 140 mAh g−1 (∼85 % of its specific capacity at room temperature) at −60 °C and 0.2 C. This study provides a practical guidance of the design of LIBs with outstanding rate performances and low temperature resistance.