ABSTRACT:0D hybrid manganese halides represent an emerging class of luminescent materials, yet their practical application has been hindered by the intrinsic trade-off between optical performance and mechanical flexibility. Here, a green synthesis of 0D (ECMP)₂MnBr₄ crystal is reported, exhibiting unprecedented triple-mode emission (photoluminescence, X-ray scintillation, and mechanoluminescence) through rationally designed highly symmetric [MnBr4]₂− tetrahedra, achieving near-unity photoluminescence quantum yield (98.97%), record-low X-ray detection limit (15.62 nGy_air s⁻¹)and multi-stimuli responsiveness (rubbing, squeezing, stretching). The material’s ultralow electron-phonon coupling (S = 1.438) and defect-suppressing Π-Π stacking enable exceptional environmental stability and closed-loop recyclability via solvent-mediated recrystallization. Innovatively, (ECMP)₂MnBr₄ is first integrated into thermoplastic polyurethane via wet-spinning, simultaneously retaining single-crystal emission intensity and achieving remarkable elasticity (>1000% strain) for deformation-resistant wearable applications. This work establishes a new design paradigm for sustainable multifunctional optoelectronics, with immediate applications in wearable displays, high-resolution X-ray imaging, and self-powered optical sensors.