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Separators are becoming increasingly important in both academic research and industrial production as a means of enhancing the performance of lithium‐ion batteries (LIBs), particularly at a high rate. However, fast charge–discharge processes will produce local heat accumulation, which accelerates the local reaction rate of Li+ to form lithium dendrites. Commercial polyolefin separators fail to tackle the above issue due to inferior thermal stability. Herein, a core–shell structure is proposed to reinforce the polyvinylidene fluoride‐hexafluoropropylene (PVDF‐HFP) matrix through encircling carbon nanotube (CNT) by adherent polydopamine (PDA). The core–shell 3D structure with PDA avoids the short circuits caused by the electrically conductive CNT, and meantime, the CNT serves as an effective radiator for dispersing local heat sources verified through finite element analysis. The composite separator allows LIBs to achieve high Li+ conductivity (0.49 × 10−3 S cm−1) and Li+ transfer number (0.74), resulting in a high capacity retention of 87.35% after 800 cycles at 5C. In particular, the safety is confirmed that the composite separator avoids violent growth of lithium dendrites caused by local heat accumulation through phase‐field simulations. This work suggests a promising approach for the fabrication of core–shell nanotube composite separators for high‐rate and safe LIBs. [ABSTRACT FROM AUTHOR]

Lithium metal batteries (LMBs) have aroused extensive interest in the field of energy storage owing to the ultrahigh anode capacity. However, strong solvation of Li+ and slow interfacial ion transfer associated with conventional electrolytes limit their long‐cycle and high‐rate capabilities. Herein an electrolyte system based on fluoroalkyl ether 2,2,2‐trifluoroethyl‐1,1,2,3,3,3‐hexafluoropropyl ether (THE) and ether electrolytes is designed to effectively upgrade the long‐cycle and high‐rate performances of LMBs. THE owns large adsorption energy with ether‐based solvents, thus reducing Li+ interaction and solvation in ether electrolytes. With THE rich in fluoroalkyl groups adjacent to oxygen atoms, the electrolyte owns ultrahigh polarity, enabling solvation‐free Li+ transfer with a substantially decreased energy barrier and ten times enhancement in Li+ transference at the electrolyte/anode interface. In addition, the uniform adsorption of fluorine‐rich THE on the anode and subsequent LiF formation suppress dendrite formation and stabilize the solid electrolyte interphase layer. With the electrolyte, the lithium metal battery with a LiFePO4 cathode delivers unprecedented cyclic performances with only 0.0012% capacity loss per cycle over 5000 cycles at 10 C. Such enhancement is consistently observed for LMBs with other mainstream electrodes including LiCoO2 and LiNi0.5Mn0.3Co0.2O2, suggesting the generality of the electrolyte design for battery applications. [ABSTRACT FROM AUTHOR]