Nanostructured ceria doped with other rare earth elements is a good oxygen ion conductor, which gives rise to various catalytic applications such as the construction of membranes for syngas production by partial oxidation of methane. This article focuses on the Gd-doped cerium dioxides, which can be modified with Pt or Pd to enhance the reactivity of the lattice oxygen in interaction with methane. The aim of the work is the elucidation of correlations between the structural, electronic, and chemical properties of these nanomaterials. Detailed studies were performed for a series of samples with and without surface modification by noble metals using a complex combination of physicochemical methods: XRD, TEM, CH(4) TPR, XPS, SIMS, and FTIR spectroscopy of adsorbed CO. XPS and TPR data revealed that surface modification with noble metals enhances the reducibility of the doped ceria support, where the effect is more pronounced for Pd than for Pt. The formation of highly cationic Pd species due to strong metal support interactions provides a possible explanation for this behavior. Furthermore, the results obtained in the present work for the Gd-doped ceria system are compared to those obtained previously for the Pr-doped ceria system.