Ma et al. Energy Mater. 2025, 5, 500029 DOI: 10.20517/energymater.2024.176 Energy Materials © The Author(s) 2025. Open Access This article is licensed under a Creative Commons Attribution 4.0 International License (https://creativecommons.org/licenses/by/4.0/), which permits unrestricted use, sharing, adaptation, distribution and reproduction in any medium or format, for any purpose, even commercially, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. www.oaepublish.com/energymater Open Access Research Highlight Full-performance coordinated design for polymer-in- salt solid electrolyte Qingyang Ma 1 , Siying Shen 1 , Jun Lu 1 , Leyan Ai 2 , Yaohui Hou 1 , Yuanyuan Li 3,* , Jinping Liu 1,* 1 School of Chemistry, Chemical Engineering and Life Science, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, Hubei, China. 2 School of Material Science and Engineering, Wuhan University of Technology, Wuhan 430070, Hubei, China. 3 School of Integrated Circuits, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China. *Correspondence to: Prof. Jinping Liu, School of Chemistry, Chemical Engineering and Life Science, State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, No. 122, Luoshi Road, Hongshan District, Wuhan 430070, Hubei, China. E-mail: liujp@whut.edu.cn; Prof. Yuanyuan Li, School of Integrated Circuits, Huazhong University of Science and Technology, No. 1037, Luoyu Road, Hongshan District, Wuhan 430074, Hubei, China. E-mail: liyynano@hust.edu.cn How to cite this article: Ma, Q.; Shen, S.; Lu, J.; Ai, L.; Hou, Y.; Li, Y.; Liu, J. Full-performance coordinated design for polymer-in- salt solid electrolyte. Energy Mater. 2025, 5, 500029. https://dx.doi.org/10.20517/energymater.2024.176 Received: 16 Sep 2024 First Decision: 12 Oct 2024 Revised: 2 Nov 2024 Accepted: 6 Nov 2024 Published: 17 Jan 2025 Academic Editor: Wei Tang Copy Editor: Fangling Lan Production Editor: Fangling Lan Solid-state lithium batteries (SSLBs) using solid electrolytes have been identified as one of the most promising next-generation energy storage devices due to their improved safety and high energy density. In particular, solid polymer electrolytes (SPEs; excluding gel polymer electrolytes and polymer electrolytes with free solvents) have been widely chosen in SSLBs due to their high lithium metal compatibility, good contact with electrodes, and more favorable manufacturing process [1-3] . Nonetheless, there are still key challenges that SSLBs with SPEs must overcome. These include low ionic conductivity (10 -7 -10 -5 S cm -1 ) at room temperature and the difficult balance among mechanical strength, ionic conductivity, and high-voltage applications for long-term cycling [4] . Polymer-in-salt solid electrolytes (PISSEs), defined as a small amount of a high-molar-mass polymer mixed with high fraction of lithium salts (generally exceeding 50 wt%), have been proposed to address the ionic conductivity issue [5] . By using PISSEs, the ionic conductivity of typical SPEs can be increased by an order of magnitude (promoted to 10 -4 S cm -1 ), since PISSEs can construct a unique Li + transport channel through the ion clusters in the system, compared with the Li + migration in ordinary SPEs that only depends on the segmental movement of the polymer matrix.