Pristine, Si-doped, and Si/Nd-codoped yttrium aluminum garnet (YAG) nanoparticles were synthesized by pyrolysis of complex compounds of aluminum and yttrium with triethanolamine. It was found that the coexistence of Si4+ and Nd3+ increased the solubility of both ions and promoted the formation of YAG phase. Single-phase, nanocrystalline Si/Nd:YAG powders were obtained at calcination temperatures as low as 920 degrees C. The optical behavior of the Si/Nd:YAG nanopowders was similar to that of single-crystal Nd:YAG.