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With the increasing application of electric vehicles, the surging of lithium-ion batteries (LIBs) may foreshadow potential environmental disruptions stemming from mishandling spent LIBs and greenhouse gas emissions from recycling. Urgent advancements are needed in the current recycling technologies for dead LIBs. Herein, we propose a solution to address the challenge of industrial LIB waste recycling by repurposing it into environmentally friendly functional materials. Specifically, unitary and ternary transition metal organic frameworks (TT-MOFs) were successfully synthesized for use in the separator for high-performance lithium-sulfur (Li-S) batteries. The unique ternary MOFs demonstrate the capability to mitigate the shuttle effect and enhance the adsorption and conversion of lithium polysulfides during cycling. Notably, we achieved an initial discharge capacity of 1008.7 mA h g–1at 0.5 C, with a decay rate of only 0.054% after 500 cycles. This research reuses waste solutions from the wet metallurgy process of LIB recycling and unveils a promising approach for the development of sustainable energy-storage materials in the future.