The　commercial　feasibility　of　lithium-sulfur　(Li-S)　batteries　is　still　hindered　by　three　long-standing　problems:　substantial　volumetric　expansion　of　sulfur　cathodes　during　cycling,　serious　polysulfide　shuttle　phenomenon,　and　sluggish　redox　kinetics.　Addressing　these　limitations　through　innovative　material　engineering,　this　study　presents　a　sustainable　approach　by　developing　a　novel　aqueous　multifunctional　binder　(designated　AG-DAA)　derived　from　aloe　vera　gel　crosslinked　with　d-aspartic　acid.　The　rationally　designed　AG-DAA　binder　demonstrates　dual　functionality　to　overcome　existing　barriers.　Mechanically,　its　superior　elastic　modulus　(1.2　GPa)　and　tensile　strength　(156　MPa)　enable　effective　accommodation　of　sulfur　cathode　volume　fluctuations,　thereby　maintaining　structural　integrity　throughout　extended　cycling.　Chemically,　the　abundant　polar　functional　groups　(-COOH,　-OH)　facilitate　three　critical　interactions:　(1)　enhanced　Li+　transport　through　enhanced　lithium　affinity,　(2)　strong　chemisorption　of　lithium　polysulfides　via　Lewis　acid-base　interaction,　and　(3)　catalytic　acceleration　of　sulfur　redox　reactions.　As　a　result,　the　AG-DAA　based　cathode　achieves　an　initial　specific　capacity　of　1130.8　mA　h　g−1　at　0.5C,　maintaining　600.3　mA　h　g−1　after　500　cycles　with　a　coulombic　efficiency　exceeding　98.7%.　Remarkably,　under　high-rate　conditions　(4C),　the　system　demonstrates　exceptional　stability　with　capacity　retention　of　51.3%　after　1000　cycles,　corresponding　to　an　ultralow　cycle　degradation　rate　of　0.049%　per　cycle　representing　a　20%　improvement　over　conventional　PVDF　binders.　This　investigation　establishes　a　paradigm　for　eco-friendly　binder　engineering　in　Li-S　battery　systems,　demonstrating　that　rational　design　of　functionalized　natural　polymers　can　simultaneously　address　multiple　electrochemical　challenges.　©　2025　The　Royal　Society　of　Chemistry.