Graphitic carbon nitride (g-C3N4) was supported on SrAl2O4:Eu,Dy-SiO2 by a colloidal-sol coating method to improve its light absorption property. Transmission electron microscopy (TEM) revealed that the nanoparticles of g-C3N4 were coated on sub-micron phosphor particles and nanoscale surface roughness was imparted by the SiO2-binder. Photoluminescence (PL) spectrum of the g-C3N4 supported on SrAl2O4:Eu,Dy exhibited a broadband emission from 400 to 650 nm. Increasing silica-binder in the g-C3N4/SrAl2O4:Eu,Dy composites suppressed the PL emission peak at 525 nm for SrAl2O4:Eu,Dy. Photocatalytic degradation activity was evaluated with 5 ppm methylene blue (MB) solutions under germicidal ultraviolet (UV) and visible (Vis) solar light illuminations. The UV/Vis photocatalytic efficiency was improved by supporting g-C3N4 on the SrAl2O4:Eu,Dy phosphor and with the addition of SiO2 as a binder. In addition, low silica addition effectively improved the adhesiveness of the g-C3N4 coating on the SrAl2O4:Eu,Dy surface. Recyclability tests of photocatalysis for the SrAl2O4:Eu,Dy-0.01M SiO2/50wt% g-C3N4 composites exhibited a remarkable stability by maintaining the degradation efficiencies above 90% in four cycles. Therefore, the composite of g-C3N4-supported SrAl2O4:Eu,Dy-SiO2 is a prospective photocatalyst activating under UV/Vis light irradiation for the elimination of environmental pollutants.