well as safety concerns if/when crossover occurs.Non-aqueous Li-based fl ow batteries utilizing organic redox compounds (e.g., ferrocene-based redox, [ 24,25 ] 2,2,6,6-tetramethylpiperidine-1-oxyl, (TEMPO)-based) [ 8,11 ] as catholytes have been shown an effective approach to increase the power density, [ 24,25 ] cycle life, [ 24,25 ] and energy density of the RFBs. [ 1,6,7,9,24,25 ] However, the low solubility of organic redox compounds has limited further improvement in energy density. Alternatively, a non-aqueous Libased semi-solid fl ow battery was proposed by Duduta et al. [ 26 ] In this concept, insoluble active materials (lithium cobalt oxide (LiCoO 2 ), [ 26 ] lithium iron phosphate (LiFePO 4 ), [ 27 ] silicon [ 28 ] ) are mixed with conducting carbon (e.g. Ketjenblack (KB)) and Li + ion supporting electrolyte to form a suspension, which permits catholyte/anolyte concentration beyond solubility limit and shows much higher achieved volumetric capacity. Along this concept, we have recently reported a sulfur/carbon (S/C) composite semi-solid fl ow battery achieving superior volumetric capacity (294 Ah L −1 catholyte ). [ 29 ] Another important emerging direction in the fi eld is applying redox reactions to mediate and facilitate intercalation or conversion reactions of energy storage materials. [30][31][32] Applying this concept, Jia et al. [ 33 ] have recently demonstrated a high-energy density all redox fl ow lithium battery reaching tank energy density ≈500 Wh L −1 (50% porosity).In this work, we propose a new concept of multiple redox semi-solid-liquid (MRSSL) fl ow battery, which takes advantage of both highly soluble active materials in the liquid phase and high-capacity active materials in the solid phase, to form a biphase MRSSL catholyte. Here, we used liquid LiI electrolyte and solid S/C composite as an example to demonstrate an LiI-S/C MRSSL catholyte, which achieved the highest catholyte volumetric capacity (550 Ah L −1 catholyte ) to date and superior energy density (580 Wh L −1 catholyte+lithium ) with high columbic effi ciency (>95%). We further show that the presence of LiI synergistically facilitates the electrochemical utilization and reduces the viscosity of the catholyte. A continuous fl ow battery system based on the LiI-S/C MRSSL catholyte is demonstrated and the infl uence of fl ow rate and current density on the battery performance will be discussed. The MRSSL concept provides wide-open opportunities for numerous combinations of solid and liquid active materials and offers a new direction for designing next-generation high-energy-density fl ow batteries.