The　separation　and　recovery　of　key　metals　are　essential　for　the　sustainable　recycling　of　spent　lithium-ion　batteries　(SLIBs).　In　this　paper,　a　three-compartment　electrolysis　is　proposed　to　achieve　the　direct　separation　of　multiple　components　in　a　one-step　process　through　the　application　of　an　electric　field.　In　the　middle　compartment,　lithium　nickel　cobalt　manganese　oxide　(NCM)　material　dissolves　and　separates　from　graphite.　Simultaneously,　Ni-Co　alloy　deposits　at　the　cathode,　while　MnO2　synthesizes　at　the　anode.　Additionally,　Li+　concentrates　and　subsequently　precipitates　as　Li2CO3　through　chemical　precipitation　in　the　electrolyte.　As　a　result,　the　leaching　efficiencies　of　Ni,　Co,　Mn,　and　Li　in　spent　lithium　nickel　cobalt　manganese　oxide　(SNCM)　materials　reach　94.30　%,　90.78　%,　98.19　%,　and　94.33　%,　respectively,　in　the　middle　compartment　within　6　h　at　80　℃.　Meanwhile,　the　recovery　rates　for　Ni,　Co,　and　Mn　are　87.22　%,　81.50　%,　and　48.89　%,　respectively.　The　proportions　of　Ni　and　Co　in　the　Ni-Co　alloy　are　33.42　%　and　44.82　%,　respectively.　Li2CO3　with　a　purity　greater　than　95　%　is　recovered　from　the　electrolyte　through　simple　concentration　and　precipitation.　For　every　1　kg　of　SNCM　electrode　powder　recovered,　the　carbon　emissions　from　the　three-compartment　electrolysis　and　electrolyte　reuse　are　3.81　kg　CO2　eq.　and　−3.47　kg　CO2　eq.,　resulting　in　economic　benefits　of　$0.25　and　$2.06,　respectively.　This　approach　enables　the　simultaneous　separation　and　recovery　of　multiple　metals　in　a　single　step,　addressing　the　growing　demand　for　critical　energy　metals.　©　2025　Elsevier　B.V.