Phase-pure [NiO](0.5)[Al2O3](0.5) spinel nanoparticles (NPs) with limited aggregation were obtained via liquid-feed flame spray pyrolysis (LF-FSP) by combusting metalloorganic precursor solutions. Thereafter "chocolate chip-like" Ni-x[NiO0.5-x][Al2O3](0.5) nanoparticles consisting of primary [NiO0.5-x][Al2O3](0.5) particles with average particle sizes of 40-60 nm decorated with Ni metal particles (<10 nm in diameter) dispersed on the surface were synthesized by heat treating the spinel NPs at 800 degrees C/7 h in flowing 5% H-2:N-2 100 mL/min in a fluidized bed reactor. The synthesized materials were characterized using TEM, XRD, FTIR, and TGA/DTA. The Ni depleted areas consist primarily of gamma-Al2O3. The Ni content (800 degrees C) was determined by TGA to be approximate to 11.3 wt.% based on TGA oxidation behavior. The successful synthesis of such nanocomposites with limited aggregation on a high temperature support provides a facile route to synthesize well-defined NP catalysts. This work serves as a baseline study for an accompanying paper, wherein thin, flexible, dense films made from these same NPs are used as regenerable catalysts for carbon nanotube syntheses.