Photoluminescence and coloring properties of Tb3+-doped Y2BaMO5 (M=Cu, Zn) were investigated for developing an inorganic luminescent pigment. Powder samples were synthesized by three kinds of methods, namely, a simple solid-state reaction, a stepwise solid-state reaction, and a precipitation. Y2BaZnO5:Tb3+ obtained by the simple solid-state reaction showed green emissions under UV light irradiation. However, substitution of Cu2+ for Zn2+ to give the material a green color led to the quenching of the green emissions from Tb3+. The distance between Tb3+ and Cu2+ was assumed to play a crucial role in luminescence behavior due to the occurrence of Tb3+-Cu2+ energy transfer in this system. We then changed the synthesis method from the conventional solid-state reaction to the precipitation method based on solution chemistry. In this latter method, green-colored, green-luminescent phosphors could be obtained successfully because the coloring Cu2+ ions and the emitting Tb3+ ions were separated in the particle.