A computational evolutionary optimization process is adopted to screen a Eu3+‐doped alkali earth borosilicate system in an attempt to search for red phosphors with a high luminescent efficiency when excited by soft ultraviolet irradiation. The evolutionary optimization process involves a genetic algorithm and combinatorial chemistry, which was tailored for the development of light‐emitting diode (LED) phosphors. Vertical simulations and an actual synthesis have been carried out in the present investigation, and promising red phosphors for three‐band white LED applications have been obtained.