The development of polymer electrolytes with good ion transport capacity and high mechanical strength is a big challenge for solid polymer electrolytes.

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Solid polymer electrolytes (SPEs) are still being considered as a candidate to replace liquid electrolytes for high‐safety and flexible lithium batteries due to their superiorities including light‐weight, good flexibility, and shape versatility. However, inefficient ion transportation of linear polymer electrolytes is still the biggest challenge. To improve ion transport capacity, developing novel polymer electrolytes are supposed to be an effective strategy. Nonlinear topological structures such as hyperbranched, star‐shaped, comb‐like, and brush‐like types have highly branched features. Compared with linear polymer electrolytes, topological polymer electrolytes possess more functional groups, lower crystallization, glass transition temperature, and better solubility. Especially, a large number of functional groups are beneficial to dissociation of lithium salt for improving the ion conductivity. Furthermore, topological polymers have strong design ability to meet the requirements of comprehensive performances of SPEs. In this review, the recent development in topological polymer electrolytes is summarized and their design thought is analyzed. Outlooks are also provided for the development of future SPEs. It is expected that this review can raise a strong interest in the structural design of advanced polymer electrolyte, which can give inspirations for future research on novel SPEs and promote the development of next‐generation high‐safety flexible energy storage devices.

Lithium metal batteries hold promise for energy storage applications but suffer from uncontrolled lithium dendrites. In this study, a new composite membrane based on modified natural polymer and ZIF‐67 is designed and prepared by the in situ composite method for the first time. Among them, a modified natural polymer composed of lithium alginate (LA) and polyacrylamide (PAM) can be obtained by electrospinning. Importantly, the polar functional groups of natural polymers can interact by hydrogen bonding and MOFs can construct lithium‐ion transport channels. Consequently, compared with LA‐PAM electrolyte without MOF, the electrochemical stability window of ZIF‐67‐LA‐PAM electrolyte becomes wider from 4.5 to 5.2 V, and the lithium‐ion transference number ( t Li+ ) enhances from 0.326 to 0.627 at 30°C. It is worth noting that the symmetric cells with ZIF‐67‐LA‐PAM have superior stable cycling performance at 40 and 100 mA cm −2 , and a high rate at 10C and 20C for LFP cells. Besides, the cell with NCM811 high‐voltage cathode can run stably for 400 cycles with an initial discharge capacity of 136.1 mAh g −1 at 0.5C. This work provides an effective method for designing and preparing MOF‐natural polymer composite electrolytes and exhibits an excellent application prospect in high‐energy‐density lithium metal batteries.

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