The pyrolysis of organometallic clusters containing osmium and/or ruthenium on a silica support leads to metallic nanoparticles in the 1 to 10 nm size range. The particle size obtained is correlated to the ligand set, and there are also indications that the shape of the cluster may have some effect on the shape of the nanoparticles obtained. In comparison, the size of nanoparticles obtained through thermolysis in a coordinating solvent are fairly independent of the nature of the organometallic precursor and tends to lead to aggregation of smaller, spherical nanoparticles into larger particles.