A facile, but effective, two-step method was developed to prepare monoclinic LaPO4:Eu3+ microspheres composed of microprisms with a controllable morphology. XRD and SEM studies revealed a spherical morphology and crystalline structure for the resulting material. It was also found that LaPO4:Eu3+ microspheres prepared at 800 °C showed a higher luminescent intensity than primary hexagonal LaPO4:Eu3+ microprisms. Furthermore, the luminescent performance of LaPO 4:Eu3+ microspheres was demonstrated to reach the standards of the LaPO4:Eu3+ bulk material under the same conditions. These results suggest possibilities for the use of as-synthesized monoclinic LaPO4:Eu3+ microspheres as alternatives to replace intrinsically uneven bulk materials for many application areas, including light display systems and optoelectronic devices.