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Two types of layered sulfido stannates or a molecular cluster compound are obtained upon ionothermal treatment of the simple sulfido stannate salt K 4 [SnS 4 ]    · 4H 2 O that is based on binary tetrahedral [SnS 4 ] 4−  anions. The formation of the respective products, novel compounds (C 4 C 1 C 1 Im) 2 [Sn 3 S 7 ] ( 1 a ), (C 4 C 1 C 2 Im) 2 [Sn 3 S 7 ] ( 1 b ), and (C 4 C 1 C 2 Im) 2 [Sn 4 S 9 ] ( 2 ) with layered anionic substructures, or the recently reported compound (C 4 C 1 C 1 Im) 4+x [Sn 10 O 4 S 16 (SMe) 4 ][An] x  ( A ) comprising a molecular cluster anion, is controlled by both the choice of the ionic liquid cation and the reaction temperature. We report the scale‐up of the syntheses by a factor of 100 with regard to other reported ionothermal syntheses of related compounds, and a procedure of how to isolate them in phase‐pure form – both being rare observations in chalcogenido stannate chemistry in ionic liquids. Moreover, the synthesis of compound  1 a  can be achieved by rapid cation exchange starting out from  1 b , which has not been reported for organic cations in any chalcogenido stannate salt to date.

Ionic Liquid‐Driven Formation of and Cation Exchange in Layered Sulfido Stannates – a CH 2 Group Makes the Difference