The Eu and Dy doped borophosphosilicate glass-ceramics prepared using melt quenching technique are investigated for light-emitting diode applications. The X-ray diffraction results show that the precipitation of AlPO4 crystals in glass matrix occurred during the melt quenching process, leading to the formation of glass-ceramics. The content of AlPO4 crystals depends on the B2O3/P2O5 relative content in glass matrix composition. The spontaneous conversion of Eu3+ to Eu2+ takes place in the as-obtained glass-ceramics without using reducing atmosphere during the preparation process. The conversion extent of Eu3+ to Eu2+, optical properties and structure of the as-obtained materials are related to the B2O3/P2O5 relative content. The Eu/Dy co-doped borophosphosilicate glass-ceramics display the emission bands in the blue, yellow, and red light regions and their combinations generate near white light-emission. In addition, the tunable light emission can be realized by changing the concentration of Eu and B2O3/P2O5 relative content. The as-developed Eu and Dy doped borophosphosilicate glass-ceramics show promising prospects in light-emitting diode applications.