Zero‐dimensional (0D) structure‐based manganese metal halides (MHs) are believed to be the most promising candidates for the next‐generation X‐ray scintillators due to their intense radioluminescence and environmental friendliness. However, low‐temperature (<180 °C), large‐area integration with more efficient X‐ray detection remains a tremendous challenge. Herein, from the perspective of cation (ionic liquids) structure design, the basic physical parameters of 0D MHs are regulated. And the calculations and experimental results demonstrate larger‐size cations that induce lower melting temperatures, larger exciton‐binding energies, larger ion migration energy, and tunable hardness, which are most desirable for MHscintillators. As a result, the champion materialHTP2MnBr4is achieved as glassy transparency wafer by low‐temperature (165 °C) melt‐quenching. Its application to X‐ray imaging features high spatial resolution (17.28 lp mm−1), scalability (>30 × 30 cm2), and integration with strong coupling force. Furthermore, HTP2MnBr4 glass with reproducible properties demonstrates a high light yield (38 000 photon MeV−1), excellent irradiation stability, and low detection limit (0.13 µGy s−1). The authors believe this work will provide guidance for MHscintillators to further commercial applications.