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Abstract Over recent years, Mn(II)‐organic materials showing circularly polarized luminescence (CPL) have attracted great interest because of their eco‐friendliness, cheapness, and room temperature phosphorescence. Using the helicity design strategy, herein, chiral Mn(II)‐organic helical polymers are constructed featuring long‐lived circularly polarized phosphorescence with exceptionally high g lum and Φ PL magnitudes of 0.021% and 89%, respectively, while remaining ultrarobust toward humidity, temperature, and X‐rays. Equally important, it is disclosed for the first time that the magnetic field has a remarkably high negative effect on CPL for Mn(II) materials, suppressing the CPL signal by 4.2‐times at = 1.6 T. Using the designed materials, UV‐pumped CPL light‐emitting diodes are fabricated, demonstrating enhanced optical selectivity under right‐ and left‐handed polarization conditions. On top of all this, the reported materials display bright triboluminescence and excellent X‐ray scintillation activity with a perfectly linear X‐ray dose rate response up to 174 µGy air s −1 . Overall, these observations significantly contribute to the CPL phenomenon for multi‐spin compounds and promote the design of highly efficient and stable Mn(II)‐based CPL emitters.
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