An in situ deposition procedure was developed for the nanopeapod (NPP) formation of NiAu nanoparticles inside preformed acid-exchanged hexaniobate nanoscrolls (HNB). Metal salt precursors of Ni(acac)2 and HAuCl4∙3H2O were reduced in solution under mild synthetic conditions in the presence of the preformed acid-exchanged hexaniobate nanoscrolls. Two of the surfactants used for the formation of the nanoparticles were oleylamine and triphenylphosphine oxide (TTPO). Reaction conditions were studied and modified to produce well-defined NiAu@HNB NPP systems, with monodispersed particles evenly filling and orienting within the nanoscrolls. The synthetic parameters studied were both time and temperature, with the most well-defined peapod systems being those produced from lower temperatures (100°C) and longer reaction times (60 minutes). NiAu@HNB NPPs synthesized under these conditions yielded a narrow size distribution of NiAu nanoparticles, ranging ~ 4 – 10 nm in diameter, evenly filled and oriented within the inner diameter of hexaniobate nanoscrolls (ranging ~2 μm in length).