TEM photographs were obtained on a JEOL 2010 microscope operated at 200 kV. XRD patterns were obtained on a Bruker D4 X-ray diffractometer using Cu Ka radiation. Nitrogen adsorption±desorption isotherms were acquired using a Micromeritics Tristar 3000 system at 77 K. Metal or semiconductor nanoparticles are of great interest with respect to their applications as catalysts, [1] as well as in sensors and optical [2] and electronic [2] devices. Their properties depend on the size of the nanoparticles. Thus, the accurate control of the particle size is very important for these applications. Nanoparticles have been synthesized by the oxidation or reduction of precursors.[3] Micelles [4] and stabilizing polymers [5] have also been used to restrict particle aggregation. Porous materials have been used as hosts for the synthesis of nanoparticles.[6±10] The synthesis of nanoparticles using porous materials with uniform pore sizes and high surface area as hosts has attracted interest because the sizes of the nanoparticles can be easily controlled in well-defined matrices. Mesoporous (pore size 2±50 nm) silica, FSM-16, [6] MCM-41, [7] SBA-15 [8] have been used for the synthesis of nanoparticles of Pt, Pd, Rh, Au, and Ag. A microporous (pore size < 2 nm) host, zeolite, can also be used for the synthesis of metal carbonyl clusters, [9] which takes a few days for the synthesis in a liquid-phase solvent, [9] and the reduction process generates larger particles on the external surface. These are due to the limitation of mass transfer in the liquid solvent and difficulty in controlling the growth rate of the nanoparticles from salt-type precursors, even though they are smaller than other types of precursors such as organometallic molecules. A filtration process using the vapor phase, such as chemical vapor deposition (CVD), is a very effective method for preparing particles or thin films on a nanometer scale. However, the precursors are limited in terms of high volatility and thermal stability. Conventional methods of preparing nanoparticles in porous matrices often yield nanoparticles of various sizes in the internal pores and on the external surface of the porous matrices. [8,10] Accurate size control of nanoparticles using porous materials as hosts with a wide range of uniform pore sizes, including micropores, and the investigation of the relationship between particle size and their properties still remain challenging. Supercritical fluids [11] (SCFs) have excellent properties of non-cohesivity, high diffusivity, and controllable solubility. Thus, SCFs are expected to overcome the previously men-