<p>Chiral organic-inorganic hybrid metal halides (OIHMHs) have emerged as multifunctional materials with remarkable structural diversity and chiroptical properties. Despite significant progress, current chiral OIHMHs predominantly exhibit circularly polarized luminescence (CPL) in the visible spectrum, whereas achieving ultraviolet and near-infrared (NIR) CPL remains challenging. Herein, we report a series of lead-free chiral zero-dimensional (0D) OIHMHs, (<i>R</i>/<i>S</i>-DACH)₂In₂Br₁₀:Sb³⁺/Yb³⁺ (DACH = 1,2-diaminocyclohexane), featuring spectrally tunable CPL emissions covering the visible to NIR regions. Single-crystal X-ray diffraction analysis combined with circular dichroism and CPL spectroscopy revealed that robust hydrogen-bonding interactions between organic cations and inorganic emitters in the structure play a crucial role in the chirality expression of the hybrid halides. The Sb³⁺-doped (<i>R</i>/<i>S</i>-DACH)₂In₂Br₁₀ single crystals (SCs) exhibited intense broadband emission at 644 nm, originating from the radiative transition of Sb³⁺ ions from ³P₁ to ¹S₀. This emission achieved a record photoluminescence quantum yield of 49.9% (two orders of magnitude higher than that of pristine crystals) and a luminescence dissymmetry factor (<i>g</i>_lum) of ±7.1×10⁻³. Notably, Sb³⁺/Yb³⁺ co-doped (<i>R</i>/<i>S</i>-DACH)₂In₂Br₁₀ SCs simultaneously generated dual-band CPL emissions at 644 nm (<i>g</i>_lum = ±2.1×10⁻²) and 994 nm (<i>g</i>_lum = ±6.8×10⁻³), representing an important example of NIR-CPL activity realized in OIHMHs. The fabricated LED device based on (<i>R</i>-DACH)₂In₂Br₁₀:2.7%Sb³⁺ SCs exhibited bright orange emission with a color-rendering index of 78.4, along with excellent spectral and operational stabilities. These findings not only establish a unique design strategy for tailoring broadband CPL but also expand the application potential of chiral metal halides in advanced optoelectronic technologies.</p>