Immobilized noble metal nanoparticles are being explored for a variety of applications where control over the particle size and separation distance on the substrate is important for performance. A proof of concept is presented that Au nanoparticles can be deposited in a single step with control over the size and separation distributions using an aerosol process. Samples were deposited with mean particle diameters in the range from 15 to 43 nm, and mean separation distances from 11 to 39 nm. Depending on the separation distance, particles exhibited localized surface plasmon resonance dominated by either intra- or interparticle resonances, as determined by ultraviolet-visible extinction spectroscopy. Ultrathin TiO2 shells of different thicknesses, in the range from 0 to 24 nm, were deposited on the Au nanoparticles by atomic layer deposition to determine the sensing distance into the surrounding dielectric medium for these materials, which was estimated to be 10 nm.