Sm3+-doped SrO-Al2O3-SiO2 glass-ceramics with excellent luminescence properties were prepared by batch melting and heat treatment. The crystallization behavior and luminescent properties of the glass-ceramics were investigated. The results indicate that the crystal phase in this system is monocelsian (SrAl2Si2O8). Under the excitation with blue light (475 nm) the Sm3+-doped SrO-Al2O3-SiO2 glass-ceramics emit green, orange and red lights centered at 565, 605, 650 and 715 nm, which can be assigned to the (4)G(5/2) -> H-6(J/2) (J = 5, 7, 9, 11) electron transitions in Sm3+ ions, respectively. With the increase of nucleation/crystallization temperature, the crystallite part rises from 66 to 79%. Besides, by increasing crystallization temperature or concentration of Sm3+, the samples emission located at 565, 605 and 650 nm is intensified significantly. We envision that, by fine controlling and combining of these three (green, orange and red) lights in an appropriate proportion, the Sm3+-doped glass-ceramics are promising luminescence materials for white light-emitting diodes devices.