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Designing phosphors that are excited by blue light is extraordinarily important for white light-emitting diodes (w-LEDs). In the present study, a new Ruddlesden–Popper type of SZO:<i>x</i>Eu³⁺ (<i>x</i> = 0.01~0.10) phosphors was developed using solid-state reactions. Interestingly, a Eu³⁺ doping-induced phase transformation from the Sr₃Zr₂O₇ (cubic) to the SrZrO₃ (orthorhombic) phase was observed, and the impact of the occupied sites of Eu³⁺ ions on the lifetime of Sr₃Zr₂O₇:<i>x</i>Eu³⁺ phosphors is discussed in detail. Diffuse reflectance spectroscopy results showed that the band gap of SZO:<i>x</i>Eu³⁺ phosphors gradually increased from 3.48 eV for undoped Sr₃Zr₂O₇ hosts to 3.67 eV for SZO:0.10Eu³⁺ samples. The fluorescence excitation spectrum showed that ultraviolet (300 nm), near-ultraviolet (396 nm) and blue light (464 nm) were all effective excitation pump sources of Sr₃Zr₂O₇:<i>x</i>Eu³⁺ phosphors, and the strongest emission at 615 nm originated from an electric dipole transition (⁵D₀→⁷F₂). CIE coordinates moved from orange (0.5969, 0.4267) to the reddish-orange region (0.6155, 0.3827), and the color purity also increased. The fabricated w-LED was placed on a 460 nm chip with a mixture of YAG:Ce³⁺ and SZO:0.1Eu³⁺ samples and showed “warm” white light with a color rendering index (CRI) of 81.8 and a correlation color temperature (CCT) of 5386 K, indicating great potential for application in blue chip white LEDs.