Lithium-sulfur (LiS) batteries are considered to be the most promising energy storage system to replace lithium-ion batteries due to their ultra-high energy density. However, the shuttling of polysulfides and the growth of lithium dendrites lead to several challenges for practical use. This study, UIO-67 separator modified material coating with zwitterionic of ethyl viologen halides (EV2+2X−, X = Cl, Br, I) is prepared by a simple one-step method. The cation (EV2+) can adsorb polysulfides through electrostatic interaction, and then promote the conversion of polysulfides. The free halogen anions contribute to the desolvation of Li+ by coordination, thereby accelerating the transport of Li+. Among them, the UIO-67@EV2+2I− modified separator exhibits the best electrochemical performance for LiS batteries. The capacity decay rate is 0.022 % after 800 cycles at 2C, and it still has excellent cycle stability under high sulfur loading of 5 mg cm−2 and lean electrolyte of E/S = 3 μL mg−1. This work sheds new light on the selection of modified materials for LiS battery separators.