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The bis(fluorosulfonyl)imide anion N(SO2F)2- (i.e., FSI-) (also referred to as bis(fluorosulfonyl)amide (i.e., FSA-) and imidodi(sulphuryl fluoride)) has attracted tremendous interest in recent years for its utility in both lithium salts and ionic liquids for battery electrolyte applications. To facilitate the understanding of the characteristics of this anion, crystal structures are reported here for the uncoordinated anion in LiFSI-based solvates with cryptand CRYPT-222 and tetraglyme (G4). These crystalline solvates were analyzed by Raman spectroscopy to aid in assigning the Raman bands to the modes of ion coordination found in liquid electrolytes. These structures, as well as a thorough review of other relevant crystallographic data, provide insights into the rather remarkable properties of the FSI- anion with regard to solvate formation and electrolyte properties.