With　the　vigorous　development　of　the　new　energy　industry,　the　use　of　lithium-ion　batteries　(LIBs)　is　growing　exponentially,　and　the　recycling　of　spent　LIBs　has　gradually　become　a　research　hotspot.　Currently,　recycling　both　cathode　and　anode　materials　of　LIBs　is　important　to　environmental　protection　and　resource　recycling.　This　research　reports　a　method　of　efficient　purification　and　high-quality　regeneration　of　graphite　from　spent　LIBs　by　surfactant-assisted　methanesulfonic　acid　(MSA).　Under　the　optimal　conditions　(0.006　mol/L　sodium　dodecyl　sulfonate,　0.25　mol/L　MSA,　10　vol%　hydrogen　peroxide,　liquid–solid　ratio　of　30:1　mL/g,　60　°C,　1.5　h),　the　purity　of　the　regenerated　graphite　was　99.7　%,　and　the　recovery　efficiency　was　98.0　%.　The　regenerated　graphite　showed　the　characteristics　of　small　interplanar　spacing,　high　degree　of　graphitization,　a　small　number　of　surface　defects,　and　excellent　pore　structure,　which　was　closer　to　commercial　graphite.　Furthermore,　the　regenerated　graphite　electrode　exhibited　superior　rate　performance　and　cycling　stability　with　a　high　specific　capacity　of　397.03　mAh/g　after　50　cycles　at　0.1C　and　a　charge–discharge　efficiency　of　99.33　%.　The　recovery　of　anode　graphite　beneficial　for　resource　utilization,　environmental　protection,　and　cost　control　throughout　the　entire　production　chain.　©　2024　Elsevier　Ltd