Currently,　lithium-ion　batteries　have　an　increasingly　urgent　need　for　high-performance　electrolytes,　and　additives　are　highly　valued　for　their　convenience　and　cost-effectiveness　features.　In　this　work,　the　feasibilities　of　fullerenes　and　fluorinated　fullerenes　as　typical　bis(fluorosulfonyl)imide/1,2-dimethoxymethane　(LiFSI/DME)　electrolyte　additives　are　rationally　evaluated　based　on　density　functional　theory　calculations　and　molecular　dynamic　simulations.　Interestingly,　electronic　structures　of　C60,　C60F2,　C60F4,　C60F6,　1-C60F8,　and　2-C60F8　are　found　to　be　compatible　with　the　properties　required　as　additives.　It　is　noted　that　that　different　numbers　and　positions　of　F　atoms　lead　to　changes　in　the　deformation　and　electronic　properties　of　fullerenes.　The　F　atoms　not　only　show　strong　covalent　interactions　with　C　cages,　but　also　affect　the　C-C　covalent　interaction　in　C　cages.　In　addition,　molecular　dynamic　simulations　unravel　that　the　addition　of　trace　amounts　of　C60F4,　C60F6,　and　2-C60F8　can　effectively　enhance　the　Li+　mobility　in　LiFSI/DME　electrolytes.　The　results　expand　the　range　of　applications　for　fullerenes　and　their　derivatives　and　shed　light　on　the　research　into　novel　additives　for　high-performance　electrolytes.　©　2024　by　the　authors.