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Low-dimension perovskite materials have attracted wide attention due to their excellent optical properties and stability. Herein, Sb3+-doped Cs2ZrCl6crystals are synthesized by a coprecipitation method in which Sb3+ions partially replace Zr4+ions. The Cs2ZrCl6:xSb3+powder shows blue and orange–red emissions under a 254 and 365 nm light, respectively, due to the [ZrCl6]2–octahedron and [SbCl6]3–octahedron. The photoluminescence quantum yield (PLQY) of Cs2ZrCl6:xSb3+(x= 0.1) crystals is up to 52.5%. According to experimental and computational results, the emission mechanism of the Cs2ZrCl6:xSb3+crystals is proposed. On the one hand, a wide blue emission with a large Stokes shift is caused by the self-trapping excitons of [ZrCl6]2–octahedra under a 260 nm excitation. On the other hand, the luminescence mechanism of [SbCl6]3–octahedron is divided into two parts: 1P1→ 1S0(490 nm) and 3P1→ 1S0(625 nm). The broad-band emission, high PLQY, and excellent stability endow the Cs2ZrCl6:xSb3+powders with the potential for the fabrication of white light-emitting diodes (WLEDs). A WLED device is fabricated using a commercial 310 nm NUV chip, which shows a high color rendering index of 89.7 and a correlated color temperature of 5333 K. In addition, the synthesized Cs2ZrCl6:xSb3+crystals can be also successfully used for information encryption. Our work will provide a deep understanding of the photophysical properties of Sb3+-doped perovskites and facilitate the development of Cs2ZrCl6:xSb3+crystals in encrypting multilevel optical codes and WLEDs.