A major driving force to the study of the interaction between H 2 and cerium oxides lies in elucidating their catalytic properties. Those can be modified by the accessibility of the hydrogen reservoir in the vicinity of the active site, which is potentially achieved by the presence of cerium hydrides within what has been recently referred to as "symbiotic CeH 2+x /CeO 2 catalysts". In this work, hydrogen exposure of cerium metal surfaces, covered by a thin native oxide overlayer, results in hydrogen incorporation within the oxide and the development of hydride growth centers underneath it. Partially reacted surfaces were investigated by Raman scattering spectroscopy and X-ray diffraction. The emergence of an ∼1005 cm −1 Ce−H local vibrational mode is revealed, while proposedly forming a CeO 2−x H y oxyhydride layer on top of the CeH ∼2 hydrides that form the growth centers. The local vibrational mode attribution is substantiated by the 2 isotopic effect of the band frequency when, instead of H 2 , the metal was reacted with D 2 . Monitoring the spatial dependence of its Raman intensity across growth centers with different radii provides a spectroscopic indicator to the pulverization of their brittle hydride interior, as it accompanies the concurrent rupture of the thin overlayer. The average hydride density, which is associated with the extent of pulverization, is extracted by estimating the volume of isolated growth centers, with radii of 65−450 μm. An estimated average packing density, for a large growth center with a radius of ∼450 μm, reached ∼50% relative to that of the bulk CeH 2 .