Low-dimensional organic-inorganic hybrid metal halides have emerged as broadband light emitters for phosphor-converted white light-emitting diodes (WLEDs). Herein, we report a new zero-dimensional (0-D) lead-free metal halide (PMA)(3)InBr6 [PMA(+): (C6H5CH2NH3)(+)] that crystallizes in the monoclinic system with P2(1)/c space group. The structure consists of slightly distorted [InBr6](3-) octahedra surrounded by organic PMA(+) cations. The direct band gap characteristic of (PMA)(3)InBr6 was demonstrated by density functional theory calculation, and its relatively wide band gap of 3.78 eV was experimentally determined. Upon 365 nm ultraviolet light excitation, (PMA)(3)InBr6 exhibited strong broadband orange luminescence with a full-width at half- maximum of similar to 132 nm resulting from self-trapped exciton emission, and the photoluminescence quantum yield was determined to be similar to 35%. A WLED fabricated by combining the orange-emitting (PMA) 3 InBr 6 , a green phosphor Ba2SiO4:Eu2+, and a blue phosphor BaMgAl10O17:Eu2+ exhibited a high color-rendering index of 87.0. Our findings indicate that the organic-inorganic hybrid (PMA)(3)InBr6 may have potential for luminescence-based applications.