AbstractLead‐free halide perovskites (LHP) have attracted extensive attention in the field of next‐generation solid‐state lighting. However, single perovskite phosphor with tunable white‐light emission and ultra‐high photoluminescence quantum yield (PLQY) are rare. Here, the tunable dual‐color emission LHP phosphor is developed with a near‐unity PLQY of 99.5%. The LHP phosphor comprises Cs2NaInCl6: Sb3+/Bi3+ and Cs2InCl5·H2O: Sb3+/Bi3+ crystals, with the transition between these two perovskite structures being adjustable by the concentration of Na+. The addition of NaCl inhibits the hydrolysis of the [Sb(H2O)Cl5]2− octahedron, resulting in 3D connected [SbCl6]3− octahedron with less Jahn‐Teller distortion, and the PLQY of LHP is greater than 90%. Finally, the white‐light diode device is fabricated by assembling the LHP with a ultraviolet light‐emitting diode chip and the white light‐emitting diode device achieved Commission Internationale de l'Eclairage color coordinates of (0.34, 0.33), correlated color temperature of 4936 K, and a high color rendering index of 92.9. The LHP perovskite exhibited multimodal luminescence when excited by 365, 335, and 310 nm UV light, showing the multi‐mode anti‐counterfeiting capabilities of the LHP crystals.