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Based on the strand‐like coordination polymer (CP) type  1  ∞ [Ln(BSB) 3 (py) 2 ], [BSB] − =bis‐salicylatoborate anion, mixed Eu/Tb‐containing compounds of the constitution  1   ∞  [Eu x Tb 1−x (BSB) 3 (py) 2 ] were synthesised ionothermally for a phase width of (x=0.25–0.75) and characterized regarding structure and optical properties. Previously, known only for other lanthanides, the mixed 1D−Eu/Tb‐CPs show excellent options for statistic replacement of the Ln‐cations during synthesis yielding solid solutions. The products are highly luminescent, with the chromaticity being a direct function of the amount of the respective Ln‐ions. Corresponding to an overall addition of emission intensities, the green Tb 3+  emission and the red Eu 3+  emission allow for a chromaticity control that also includes yellow emission. Control of the luminescence colour renders them suitable examples of the versatility of statistic replacement of metal ions in coordination chemistry. In addition, crystallization of [EMIm] 2 [YCl 5 (py)] illuminates possible other products of the ionothermal reactions of [EMIm][BSB] with LnCl 3  constituted by components not being part of the main CPs.

Statistic Replacement of Lanthanide Ions in Bis‐salicylatoborate Coordination Polymers for the Deliberate Control of the Luminescence Chromaticity