Abstract CaSr 2 (PO 4 ) 2 :Dy 3+ , A + (A = Li, Na and K) phosphors were prepared through high temperature solid-state reaction. Structures of as-prepared CaSr 2 (PO 4 ) 2 :Dy 3+ , A + samples agreed well with standard phase of Ca 2 Sr(PO 4 ) 2 , and the corresponding X-ray diffraction peaks were shifted to smaller 2θ values due to Sr 2+ ions occupying Ca 2+ sites. Effects of Dy 3+ concentration and charge compensator A + on the structure and luminescence properties of CaSr 2 (PO 4 ) 2 :Dy 3+ , A + phosphors were investigated in detail. Under UV excitation at 353 nm, all CaSr 2 (PO 4 ) 2 :Dy 3+ , A + samples exhibited two emission peaks at 488 nm and 580 nm, which were due to the 4 F 9/2 → 6 H 15/2 and 4 F 9/2 → 6 H 13/2 transitions of Dy 3+ ions, respectively. White light-emitting diode was fabricated by using these white-emitting single-composition CaSr 2 (PO 4 ) 2 :Dy 3+ , A + phosphors. Luminescence intensity and decay time of CaSr 2 (PO 4 ) 2 :Dy 3+ , A + phosphors were improved remarkably with the addition of charge compensators, which would promote their applications in white light-emitting diodes with near- ultraviolet chip.