We report on binary solid-solution nanoparticles (NPs) composed of Pd and Ir, which are not miscible at the equilibrium state of the bulk, for the first time, by means of a process of hydrogen absorption/desorption from core (Pd)/shell (Ir) NPs. Only 20 at% replacement with Ir atoms doubled the hydrogen-storage capability compared to Pd NPs, which are a representative hydrogen-storage material. Furthermore, the systematic control of hydrogen concentrations and the corresponding pressure in Pd and Pd-M NPs (M = Ir, Pt, Au) have been achieved based on the band filling control of Pd NPs.