LAUSR

The existing electrode materials for lithium‐ion batteries (LIBs) generally suffer from poor rate capability at low temperatures, severely limiting their applications in winter and cold climate area. Here, partially reduced TiNb24O62 (PR‐TNO) are reported that demonstrates excellent electrochemical performance in a broad temperature range, notably at low temperatures. Its crystal structure is similar to that of Ti2Nb10O29 upon partial reduction in H2. The titanium and niobium ions in PR‐TNO enable multielectron transfer, safe operation, and high Coulombic efficiencies. Benefiting from the increased electronic conductivity of the partially reduced phase and its robust crystal structure with a large interlayer spacing, PR‐TNO shows fast electron and Li+ transport, small volume change associated with Li+ storage, and notable capacitive behavior, resulting in good electrochemical performance even at very low temperatures. At −20 °C, a large reversible capacity of 313 mAh g−1 is obtained at 0.1C, reaching 83.3% of that at 25 °C. At 5C, high rate capability (58.3% of that at 0.5C) is achieved, only slightly lower than that at 25 °C (60.7%). Furthermore, PR‐TNO demonstrates excellent cyclic stability with 99.2% of the initial capacity after 1680 cycles, confirming its excellent suitability for low‐temperature LIBs.