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Developing high‐performance infrared (IR) nonlinear optical (NLO) materials is urgent but challenging due to the competition between NLO coefficient and bandgap in one compound. Herein, by coupling NLO‐active [BS3] planar units and halide‐centered polycations, six new metal thioborate halides ABa3B2S6X (A = Rb, Cs; X = Cl, Br, I) composed of zero‐dimensional [XBamRbn/Csn] polycations and [BS3] units,...