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Hybrid manganese halide has attracted much attention in the field of environment friendly ferroelectric and photo‐responsive multifunctional materials. Here, the highly efficient photoluminescent inorganic framework MnBr42− is utilized to conceive and synthesize a series of hybrid manganese bromide compounds [RQ]2MnBr4 by introducing precisely designed quasi‐spherical cations [RQ]+ (R = H, Me, Et, FEt, Q = quinuclidine). The accurate and effective modification of cations not only achieves the satisfactory ferroelectricity, but also enhances the photoluminescence quantum yield from 38.7% to 83.65%. Moreover, [FEtQ]2MnBr4 shows a highly efficient X‐ray scintillator performance, including a large range of linear response to X‐ray dose rate from 0.3 to 414.2 μGyair s−1, a high light yield of 34 438 photons per MeV, and a low detection limit of 258 nGyair s−1. This work provides an efficient strategy for the preparation of hybrid manganese halide ferroelectrics with highly efficient light‐emission and X‐ray detection. [ABSTRACT FROM AUTHOR]