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A series of well-dispersed (Ce 1- x Tb x)PO 4 (x = 0–1) microspheres, with an average diameter of ∼1.2 μm, have been originally prepared via two-phase interfacial precipitation and subsequent calcination. Characteristics of the as-synthesized and calcination products were investigated by the combined techniques of XRD, FE-SEM, TEM, FT-IR and TG-DSC. Under 275 nm excitation, tuning the emission color from blue (0.17, 0.02) to green (0.30, 0.56) was realized via varying the Tb3+ content and through Ce3+ → Tb3+ energy transfer. The optimal content of Tb3+ was found to be ∼15 at% (x = 0.15), and the energy transfer was determined to occur via electric dipole-dipole interaction. Moreover, both the emissions of Ce3+ and Tb3+ present gradually higher thermal stability with increasing Tb3+ content owing to enhanced energy transfer. The (Ce 0.85 Tb 0.15)PO 4 microspheres, which possess the highest absolute quantum efficiency (∼60.1%) across the series and excellent thermal stability (activation energy for thermal quenching of luminescence: ∼0.312 eV), may potentially serve as a single-phase green phosphor for solid-state lighting and field-emission display. Multi-color luminescent (Ce 1- x Tb x)PO 4 (x = 0–1) microspheres were successfully fabricated via gel/solution interfacial precipitation and subsequent calcination. Image 1 • (Ce 1- x Tb x)PO 4 (x = 0–1) microspheres were obtained via interfacial precipitation. • The formation mechanism of (Ce 1- x Tb x)PO 4 spheres was proposed. • Ce3+.→ Tb3+ energy transfer was analyzed to occur via dipole-dipole interaction • (Ce 0.85 Tb 0.15)PO 4 has favorable thermal stability for Tb3+ luminescence. [ABSTRACT FROM AUTHOR]