In this paper, we show the feasibility of the pulsed-laser ablation technique to grow 20–30-nm-thick, discrete and continuous coatings on particulate material systems so that the properties of the core particles can be suitably modified. Experiments were conducted with a pulsed excimer laser (λ = 248 nm, pulse duration = 25 ns) to deposit nanoparticle coatings on Al2O3 and SiO2 core particles by irradiation of Ag and Y2O3–Eu3+ sputtering targets. Structural characterization was performed with scanning electron microscopy, wavelength dispersive x-ray mapping, transmission electron microscopy, and scanning transmission electron microscopy with z-contrast.