Novel Sc2Mo3O12:Ln(3+) (Ln = Eu, Tb, Dy, Tb/Eu, Dy/Eu) phosphors have been synthesized via a one-step hydrothermal route using glycine (Gly) as a surfactant. The phosphors were characterized using X-ray diffraction (XRD), field emission-scanning electron microscopy (FE-SEM), transmission electron microscopy (TEM), photoluminescence (PL), and luminescence decays. It was found that various surfactants had a profound influence on the crystal phase, morphology and emission intensity of the final products. Furthermore, the photoluminescence of Ln(3+)-doped Sc2Mo3O12 phosphors (Ln = Eu, Tb, Dy, Tb/Eu, Dy/Eu) was studied in detail. The energy transfer of MoO42- -> Tb3+ (Dy3+) -> Eu3+ and multicolor tunable emission occurred by changing the ratio of Tb3+/Eu3+ or Dy3+/Eu3+ under single wavelength excitation. Moreover, the energy transfer mechanism from Tb3+ (Dy3+) to Eu3+ was ascribed to dipole-dipole interactions and the energy transfer efficiency from Tb3+ to Eu3+ (95.3%) was higher than that from Dy3+ to Eu3+ (87.5%). Their tunable multicolor luminescence properties make Sc2Mo3O12:Ln(3+) (Ln = Eu, Tb, Dy, Tb/Eu, Dy/Eu) phosphors suitable for many potential applications in the fields of color displays and fluorescent lamps.