A simple and unique route to synthesize nanosize Pd particles using a zeolite support including a single-site Ti oxide moiety (TS-1) under UV-light irradiation has been developed. By the photoassisted deposition (PAD) method, a Pd precursor can be deposited directly on the photoexcited tetrahedrally coordinated Ti oxide moiety within the zeolite frameworks from an aqueous solution of Pd. The subsequent reduction with H2 generates the nanosized Pd metal particles with a narrow size distribution (PAD-Pd/TS-1). Characterization by XAFS and TEM analysis revealed that the size of the metal particles depends on the preparation methods and that the smaller sizes of Pd nanoparticles were formed on the photodeposited catalysts compared with the conventionally prepared impregnated catalysts. PAD also provides PdAu bimetallic nanoparticles from an aqueous solution of mixture of PdCl2 and HAuCl4. The catalytic activities in the direct synthesis of hydrogen peroxide (H2O2) using H2 and O2 gases under atmospheric pressure were strongly dependent on the preparation method and the presence of Au atoms. Here, both deposition of PdAu onto the TS-1 moiety under UV-light irradiation was the most efficient for the above reaction. The applicability of the present catalytic system is highlighted by the one-pot reaction of phenol using PAD-Pd/TS-1 in the presence of H2 and O2, in which both Pd nanoparticles and isolated Ti oxide moieties within the frameworks participate in the formation of H2O2 and oxidation of phenol, respectively.