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Single-phase white light-emitting CaxBa(9–x)Lu2Si6O24:Eu2+/Mn2+ codoped phosphors were successfully synthesized, and their photoluminescence properties were experimentally determined. The analysis of the experimental results suggests that the partial substitution of Ba2+ ions by smaller Ca2+ ions alters the distribution of the Eu2+ luminescence center among the three available Ba2+ sites in the host lattice, which enables the emission to be efficiently tuned from blue to blue-green-yellow region. The incorporation of Mn2+ ions resulted in a red light emission at around 618 nm, through energy transfer from Eu2+ to Mn2+ ions via dipole–dipole interactions. The incorporation of Ca2+ and Mn2+ ions also resulted in improved thermal stability. The results qualify the produced CaxBa(9–x)Lu2Si6O24:Eu2+/Mn2+ composition as a potential ultraviolet-convertible white light-emitting phosphor.