Developing broad-band-emitting phosphors is very important to light-emitting diode (LED) lighting and displays. We introduced Eu 2+ to solid solutions K 2 YZr 1−y Hf y (PO 4 ) 3 with a langbeinite-type structure to prepare a series of new phosphors. In this structure, two K + sites could be occupied by Eu 2+ cations to provide two different kinds of coordination environments, leading to broad emitting bands in the range of 390−700 nm. The coordination circumstance of Eu 2+ was analyzed by Gaussian fitting and time-resolved emission spectra. Furthermore, the emitting intensity and thermal stability can be improved by modulating the crystalline field via substituting Zr 4+ by Hf 4+ . When the Zr 4+ was fully substituted by Hf 4+ , the external quantum efficiency increased by 53.75%, giving a bright cyan emission. Finally, an archetype white-LED lamp was made using cyan phosphor K 2 YHf(PO 4 ) 3 :0.04Eu, red phosphor CaAlSiN 3 :Eu 2+ , and a 365 nm LED chip, which realized an applicable color rendering index (R a = 81) and a correlated color temperature (CCT = 3792 K).