Deep　eutectic　solvents　(DESs)　as　promising　green　solvents　have　been　proposed　for　the　removal　of　SO2　from　fuel　gases.　In　this　work,　an　efficient　SO2　absorption　strategy　based　on　three　1-ethyl-3-methylimidazolium　chlorine　([EMIM][Cl])-based　DESs,　that　is,　[EMIM][Cl]-ethylene　glycol,　[EMIM][Cl]triethylene　glycol,　and　[EMIM][Cl]-acetamide　DESs,　was　investigated.　A　comparison　of　the　predicted　absorption　efficiency　via　molecular　dynamics　(MD)　and　that　obtained　from　experimental　results　is　used　to　validate　the　simulated　results.　Then,　the　interaction　energy　and　radial　and　spatial　distribution　functions　are　calculated　based　on　the　MD　simulation　results　to　provide　molecular　insights　into　the　separation　mechanism.　The　hydrogen　bonding　and　van　der　Waals　interactions　between　molecules　and　SO2　were　investigated　by　quantum　chemical　calculations.　The　results　demonstrate　that　the　anion　([Cl](-))　plays　a　significant　role　in　the　absorption　process.　As　a　further　step,　a　modeling　method　for　SO2　absorption　and　DES　recovery　based　on　Aspen　Plus　is　established.　Under　optimal　operating　conditions,　the　SO2　absorption　ratio　exceeds　99.6%,　and　the　DES　recovery　ratio　is　99.9%.　DESs,　as　a　new　type　of　absorbent,　will　provide　new　insights　for　the　sustainable　development　of　the　green　chemical　industry.