Novel one-component multifunctional phosphors with the general formula Y1.975−x Yb0.025Er x O2S:Ti0.12Mg0.04 have been prepared via sulfiding of rare-earth, titanium, and magnesium oxides in melts of different sulfur-containing compounds of alkali metals and mineralizers under an SO2 atmosphere. The phosphors combine a long afterglow with anti-Stokes luminescence and offer unique optical emission properties: yellow luminescence under cw UV excitation with a broadband afterglow around λmax = 626 nm, predominantly narrow-band green anti-Stokes luminescence with λmax = 546 nm under 0.96-μm IR excitation, and red anti-Stokes luminescence with λmax = 670 nm under 1.55-μm IR excitation. Owing to this combination of luminescent properties, the phosphors have considerable potential for practical application.