A series of mixed Hf (X) Zr1-X O-2 oxide catalysts was prepared according to a recipe that yields the monoclinic structure. The samples were examined by EXAFS spectroscopy at the Zr K and Hf L-III edges. A fitting model was used that simultaneously fits data from both edges, and makes use of an interdependent mixing parameter X (mix) to take into account substitution of the complementary atom in the nearest metal-metal shell. For XPS analysis, Scofield factors were applied to estimate the relative atomic surface concentrations of Zr and Hf. EXAFS results suggested that a solid bulk solution was formed over a wide range of X for Hf (X) Zr1-X O-2 binary oxides, and that the relative ratio was retained in the surface shell (i.e., including some subsurface layers by XPS) and the surface (e.g., by ISS). The increase in selectivity for the 1-alkene from dehydration of alcohols at high Zr content does not correlate smoothly with the tuned relative atomic concentration of Hf to Zr. The step change at high Zr content appears to be due to other indirect factors (e.g., surface defects, oxygen vacancies).