Palladium nanoparticles were immobilized within the pores of metal organic frameworks MIL-125 and amine-functionalized NH2-MIL-125 using photoassisted and ion exchange deposition methods. The resulting materials showed a very high activity for hydrogen production at ambient temperature in comparison to other titanium-based porous materials. The amine groups in NH2-MIL-125 greatly increased the H2-generating activity and acted as a stabilizer of Pd NPs. The photoassisted deposition method was a more efficient method for producing highly dispersed small NPs in the MOF materials.