In this paper, a facile one-pot molten salt electrolysis method has been proposed for the synthesis of hexagonal sheet-like Ln 2 O 2 S:Eu 3+ /Tb 3+ (Ln = Sm, La, Gd and Y) phosphors. The phase, composition, morphology, and optical properties of the phosphors were characterized by X-ray powder diffraction (XRD), high-resolution transmission electron microscope (HRTEM), and photoluminescence. The results showed that doping Eu 3+ or Tb 3+ causes no great changes to the crystal structure. Under the excitation of 394 nm light, sheet-like Ln 2 O 2 S:Eu 3+ (Ln = Sm, La, Gd, and Y) exhibited predominantly red emission at around 627 nm, which corresponds to the absorption of host crystals and the energy level transitions of 5 D 0 to 7 F 2 configuration of Eu 3+ ions. The sheet-like Ln 2 O 2 S:Tb 3+ exhibited characteristic excitation of Tb 3+ under 364 nm. The emission spectra of Ln 2 O 2 S:Tb 3+ (Ln = Sm, La, Gd, and Y) were measured, and those emission lines between 450 and 650 nm corresponded to the transitions of 5 D 4 to 7 F J (J = 0−6) ground state energy levels which belonged to the characteristic emission of Tb 3+ . The fabrication mechanism of the sheet-like Ln 2 O 2 S:Eu 3+ /Tb 3+ (Ln = Sm, La, Gd, and Y) was also investigated. This approach provides new avenues for the preparation of phosphors for applications in light-storing fields.