An evolutionary optimization process involving a genetic algorithm and combinatorial chemistry (combi-chem) was tailored exclusively for the development of LED phosphors. The genetic algorithm assisted combi-chem (GACC) is a well-known, very efficient heuristic optimization method. Therefore the combination of a genetic algorithm and combi-chem would enhance the searching efficiency when applied to phosphor screening. The ultimate goal of our study was to develop oxide red and green phosphors, which are suitable for three-band white light emitting diodes (LED). In this regard, promising red and green phosphors for three-band white LED applications, such as Eu0.14Mg0.18Ca0.07Ba0.12B0.17Si0.32Od and Tb0.01Gd0.02Ce0.04B0.1Si0.83Od, were obtained.