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Pb₂Ga₃F₆(SeO₃)₂X₃·2H₂O achieve a better balance between the large SHG effect and wide band gap in the current HTO family. 

Abstract Birefringent materials are widely used in various advanced optical systems, owing to their vital role in creating and controlling polarized light. Currently, Sn²⁺‐based compounds containing stereochemically active lone‐pair (SCALP) cations are extensively investigated and considered as one class of promising birefringent materials. To solve the problem of relatively narrow bandgap of Sn²⁺‐based compounds, alkali metals and multiple halogens are introduced to widen the bandgap during the research. Based on this strategy, four new Sn²⁺‐based halides, A₂Sn₂F₅Cl and ASnFCl₂(A = Rb and Cs), with large birefringence, short ultraviolet (UV) cutoff edge, and wide transparent range are successfully found. The birefringences of A₂Sn₂F₅Cl (A = Rb and Cs) are 0.31 and 0.28 at 532 nm, respectively, which are among the largest in Sn‐based halide family. Remarkably, A₂Sn₂F₅Cl possess relatively shorter UV cutoff edge (<300 nm) and broad infrared (IR) transparent range (up to 16.6 µm), so they can become promising candidates as birefringent materials applied in both UV and IR regions. In addition, a comprehensive analysis on crystal structures and structure–property relationship of metal Sn²⁺‐based halides is performed to fully understand this family. Therefore, this work provides insights into designing birefringent materials with balanced optical properties.