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Red-emitting Ca3−xEuxZr1−yAlySi2O9+(x−y)/2 (0.05 ≤ x ≤ 0.25, 0 ≤ y ≤ 0.07) phosphors were synthesized in a single phase form by the conventional solid-state reaction method and their photoluminescence properties were characterized. The charge-transfer efficiency from O2− to Eu3+ was controlled by the Al3+ doping into the Zr4+ site in the host Ca3ZrSi2O9 lattice, which resulted in the successful enhancement of the luminescent emission intensity of these phosphors. The highest emission intensity was obtained for Ca2.88Eu0.12Zr0.95Al0.05Si2O9.035, where the relative emission intensity of this phosphor was 94% compared with that of a commercial Y1.94Eu0.06O3 phosphor.